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夜神安卓模拟器-安卓模拟器电脑版下载_安卓手游模拟器_手机模拟器_官网

夜神安卓模拟器-安卓模拟器电脑版下载_安卓手游模拟器_手机模拟器_官网

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每个细节都值得夜神模拟器，电脑玩手游的神兵利器 立即下载 版本：7.0.5.9  2023/09/28绝大所数玩家的最优选择，提供最流畅稳定的表现 更新日志  |   Mac版   |   64位版 64位游戏的首选，如碧蓝档案，云顶之弈等   |   安卓9 高性能设备与安卓9游戏的首选，如原神等   |   安卓12测试版 全新安卓9开启更强大的安卓9引擎超强性能游戏稳定流畅，多开更尽兴极致体验轻松上手，速成手游大师

畅享手游电脑版夜神模拟器进行了全面的优化，无论是游戏还是应用，用起来都会更稳定、更流畅。除此之外更有超凡的端游操作体验，让你快人一步。 更多游戏 查看详情 查看详情 查看详情 查看详情 更好玩的安卓模拟器键鼠操控、极致多开，操作助手… 每一个功能做到极致只为您的游戏体验。 夜神模拟器，让手游更好玩。更多教程 自定义操作 完美的游戏操控，助你一路连胜 游戏多开 极致多开，快乐加倍 操作录制 轻松发育，一键搞定 多开同步器 控制多个模拟器进行相同操作，养号刷首抽必备 用户评价夜神模拟器，全球最多用户的选择 夜神模拟器玩明日方舟，两面包夹芝士！ 一只大哈鱼 首款兼容Hyper-V的模拟器 剑落千秋 市面上好用的一款模拟器，我玩的游戏这里都有《金铲铲之战》《明日方舟》，这些游戏在模拟器上大屏幕特别爽，而且还流畅不卡顿，祝夜神越来越好。 哇噻说游 电脑的运行环境相比手机要稳定很多，用夜神模拟器在电脑上玩能有效减少卡顿现象

小萝卜嘎嘣脆 崩坏学园2最新最好用的手游模拟器，推荐! 崩坏の牧羊人 NoxPlayer的热门影片 订阅频道 三分钟学会开VT，让你的模拟器提升十倍！！！ 2分钟带你了解夜神模拟器 手把手教你3分钟开Xposed框架 电脑玩手游的神兵利器立即下载 423下载站Alas碧蓝航线小助手极速下载游戏资讯攻略手游模拟器手机模拟器87G手游网浏览器家园华军软件园电视直播软件玩一玩游戏核弹头下载特玩游戏07073游戏网ZOL下载多特软件园奇游加速器手游之家手游下载biubiu加速器中国体育直播TVWin11KK录像机 240 点这里查看此应用无法在此设备上运行的解决办法~

推荐内容 【参与瓜分888元奖金】夜神创作打卡挑战 原神3.4【流程攻略】纸映成戏活动|解析攻略（终章） 阴阳师：粉婆婆|御魂搭配攻略 解忧小村落电脑版怎么玩？模拟器多开及键位设置教程 奥特曼：集结_电脑版怎么玩？模拟器多开及键位设置教程 热门游戏 原神 阴阳师 明日方舟 碧蓝航线 命运冠位指定 帮助信息 键盘操控的使用方法 模拟器安装失败解决办法 如何流畅使用夜神模拟器，避免卡顿 模拟器启动失败的解决办法（卡99%等） 游戏下载失败/设备不兼容/找不到游戏的解决办法 NOX官网 NoxGroup 关于夜神 使用场景 关于我们 加入我们 官方博客 充值说明 © 2024 yeshen.com 家长监护工程纠纷处理隐私协议用户协议 媒体报道联系我们 京公网安备 11010802020549号京网文（2018）11074-1003号京ICP证160250号京ICP备15013615号

Moni，标签管理记账的又一个选择 | App+1 - 少数派

Moni，标签管理记账的又一个选择 | App+1 - 少数派

PRIMEMatrix栏目Pi Store更多 无需申请，自由写作 任何用户都可使用写作功能。成功发布 3 篇符合基本规则的内容，可成为正式作者。了解更多退出登录反馈PRIMEMatrix栏目Pi Store更多 Moni，标签管理记账的又一个选择 | App+1主作者少数派会员了解详情 >关注李大超人Leo少数派作者少数派作者 已过九局下半 李大超人Leo关注李大超人Leo少数派作者少数派作者 已过九局下半 联合作者少数派会员了解详情 >关注李大超人Leo少数派作者少数派作者 已过九局下半 李大超人Leo关注李大超人Leo少数派作者少数派作者 已过九局下半 2017 年 01 月 29 日 在这个 App 迭代更新如此之快的时代，「老牌」这个词或许能带给用户一定的安全感，尤其是记账应用——以长时间使用的数据做为支撑。目前，虽然对新用户我一定首推 MOZE，但我自己仍然守着 MoneyWiz 不放手，这个从 2012 年就开始发家的记账 App 给我带来的安全感让我愿意舍弃一些使用体验。

Moni 也是一款老牌记账 App：2012 年发布 v1.0，2014 年发布 v2.0，2016年发布 3.0，等阶数列的刚刚好。

Moni 达不到专业级：不能设置预算、报表较为简单、不能按照层级管理分类，但是如果你不是一个对记账要求到达强迫症的级别，那么它做的正好比刚刚好再多一些。

Moni 的使用逻辑很简单——红色支出、绿色收入，除了金额之外，你还可以记录时间、分类、位置（自动定位）、和笔记，在分类管理上，Moni 采用的是标签管理方式，你可以为一笔交易选择多个标签，那些已经对 财禅 失望了的用户们可以看过来了。

它支持多账户管理，每个账户可以单独设定货币种类，除此之外，你还可以将账户、交易细节通过邮件分享给别人。此外，Moni 还提供了简单的图表向你展示收支走势，支持 Touch ID，还可以备份、导出、在多设备之间同步数据。

对我来说，Moni 最值得一说的是它的「色阶」。前文提到 Moni 的颜色逻辑是红色支出、绿色收入，它通过渐变色来提示你目前资产的净值状况：绿色为充足、黄棕色为勉勉强强、橙红色就达到警报范畴了，你可以根据你自己的经济状况设置临界值，当达到临界值时主界面就会产生相应的颜色变化。

最后，它当然有缺点。Moni 只支持英文，在中文系统下它的机翻实在可人，比如刚才的色阶，比如 Sounds Enabled 翻译成「听起来启用」（推荐打开，Moni 自己的音效听起来很舒服），并且它不支持在应用内将语言设置成英文，所以如果你是中文系统，会有一种「它在说什么？」的感觉。

另外，除了同步功能以外，最近其他跟网络连接有关系的功能都不能使用：注册账户、分享账户、自动识别位置，我已经发邮件咨询开发者，后期若有回复会在文中更新。

在更新至 3.0 版本后，原价 ￥6 的 Moni 现在完全免费且无内购，如果你对记账的要求是比刚刚好多那么一点，或者忠爱标签管理类别的话，不妨试试 Moni，你现在可以在 App Store 免费下载 Moni。415扫码分享 © 本文著作权归作者所有，并授权少数派独家使用，未经少数派许可，不得转载使用。 #应用推荐

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‎App Store 上的“Moni: Mobile Teller”

‎App Store 上的“Moni: Mobile Teller”

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Moni: Mobile Teller

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Rank Capital Inc.

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简介

Discover Moni Mobile Teller, the comprehensive financial app designed for effortless saving! As an agent, enjoy direct access to an exclusive savings account. Say goodbye to conventional limitations and embrace the freedom to save for yourself and your customers with Moni. Download today and seize control of your financial future.What does saving on Moni look like?Create a savings plan on Moni as an Agent and earn commisions.Save as low as N500 daily, weekly, bi-weekly, or monthly.Activate your Moni Wallet to fund your savings plan.Achieve multiple savings goals.Contribute your savings at no fees or charges.Enjoy instant withdrawal.Cultivate a savings habit.Enjoy instant technical support within the app.Becoming an Agent on Moni is easy. Get started in 3 steps:1. Download the Moni app2. Provide some information to set up your profile3. Register Clients and Create savings plans.

新内容

2024年1月29日

版本 1.1.1

Bug fixes and Improvements

App 隐私

开发者“Rank Capital Inc.”已表明该 App 的隐私规范可能包括了下述的数据处理方式。有关更多信息，请参阅开发者隐私政策。

与你关联的数据

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隐私处理规范可能基于你使用的功能或你的年龄等因素而有所不同。了解更多

信息

供应商

Rank Capital Limited

大小

90.4 MB

类別

财务

兼容性

iPhone

设备需装有 iOS 11.0 或更高版本。

iPad

设备需装有 iPadOS 11.0 或更高版本。

iPod touch

设备需装有 iOS 11.0 或更高版本。

Mac

需要 macOS 11.0 或更高版本以及装有 Apple M1 或更高版本芯片的 Mac。

Apple Vision

设备需装有 visionOS 1.0 或更高版本。

语言

英语

年龄分级

17+

Copyright

©️2023 Rank Capital Ltd

价格

免费

App 支持

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App 支持

隐私政策

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Moni: Savings & Loans

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更多选购方式：查找你附近的 Apple Store 零售店及更多门店，或者致电 400-666-8800。

Copyright © 2023 Apple Inc. 保留所有权利。

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Moni 簡化了亞洲品牌的電子商務管理 | MONI Group

Moni 簡化了亞洲品牌的電子商務管理 | MONI Group

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完全委外式的電商營運

我們為亞洲品牌提供完整的系統端對系統端的整合型電子商務營運與管理服務，協助他們在鎖定區域發展數位商務

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與倉儲及第三方物流合作夥伴共同管理及監控訂單履行流程

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透過全方位管理及外包的模式協助品牌節省成本

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Moni 與品牌共享專屬資源，讓品牌善用範圍廣泛的知識

降低風險

電商營運外包解決方案帶領並協助品牌快速進入市場，大幅降低風險

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我們以最新技術與最佳實務經驗協助品牌取得最新資訊

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我們在亞太地區的多個國家提供整合型的營運管理服務。我們的營運管理服務提供獨一無二的電商營運統包解決方案，支援亞洲品牌持續成長

營運及策略支援

內容及產品管理

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付款管理及會計對帳

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顧客、銷售、產品報告與分析

顧客服務

我們的多語言、多國家、多渠道和多時區的顧客服務能完全支援亞洲品牌。Moni 協助延伸品牌影響力，利用線上聊天和聊天機器人技術，強化所有溝通管道的顧客體驗

支援多國語言（英文、中文、日文、韓文、印尼文、泰文、菲律賓文、越南文）

支援多重溝通管道（電子郵件、手機、社群、線上聊天）

支援多時區，包括國定假日的自動化客服

使用聊天機器人保證回應時間及問題處理

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透過我們的客戶與合作夥伴的網路，我們提供集中化的訂單履行管理服務，與我們的營運管理服務完全整合，Moni 代表在地或區域的客戶管理訂單履行流程

訂單履行管理及監控

管理及監控訂單交貨與訂單退回

第三方物流（3PL）及倉儲管理系統（WMS）無縫系統整合

訂定標準作業流程（SOP）文件、程序與流程

行銷自動化

Moni 透過廣泛的技術合作夥伴提供行銷自動化服務，讓我們的客戶利用自動化技術，在多個渠道與國家以多語言的方式建立消費者個人化的溝通體驗。

行銷自動化程式設計與管理

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我們為客戶的電子商務網站提供後續的技術與平台支援及維護，以持續改善網站效能與最佳的正常運行時間。Moni 的專業團隊連續24小時專注於您的網站，進行例行性的維護，解決任何技術面的難題，強化各項功能，確保網站安全並維持最即時的更新

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MONI | Creating Experiences

MONI | Creating Experiences

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以體驗驅動的電子商務

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Delivering unified and connected commerce experiences that drive traffic, increase sales and strengthen customer loyalty.

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Bringing brands to life through design & ideas that elevate people’s lives to create meaningful customer experiences.

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Creating brands’ digital footprints through specialised digital and interactive production services for web and mobile.

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Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics | Nature Communications

Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics | Nature Communications

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Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics

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Published: 17 May 2017

Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics

Jian Zhang 

ORCID: orcid.org/0000-0002-0912-11971, Tao Wang2, Pan Liu 

ORCID: orcid.org/0000-0002-4063-96053,4, Zhongquan Liao5, Shaohua Liu 

ORCID: orcid.org/0000-0001-9079-53341, Xiaodong Zhuang1, Mingwei Chen3,4, Ehrenfried Zschech5 & …Xinliang Feng1 Show authors

Nature Communications

volume 8, Article number: 15437 (2017)

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ElectrocatalysisEnergy

AbstractVarious platinum-free electrocatalysts have been explored for hydrogen evolution reaction in acidic solutions. However, in economical water-alkali electrolysers, sluggish water dissociation kinetics (Volmer step) on platinum-free electrocatalysts results in poor hydrogen-production activities. Here we report a MoNi4 electrocatalyst supported by MoO2 cuboids on nickel foam (MoNi4/MoO2@Ni), which is constructed by controlling the outward diffusion of nickel atoms on annealing precursor NiMoO4 cuboids on nickel foam. Experimental and theoretical results confirm that a rapid Tafel-step-decided hydrogen evolution proceeds on MoNi4 electrocatalyst. As a result, the MoNi4 electrocatalyst exhibits zero onset overpotential, an overpotential of 15 mV at 10 mA cm−2 and a low Tafel slope of 30 mV per decade in 1 M potassium hydroxide electrolyte, which are comparable to the results for platinum and superior to those for state-of-the-art platinum-free electrocatalysts. Benefiting from its scalable preparation and stability, the MoNi4 electrocatalyst is promising for practical water-alkali electrolysers.

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IntroductionGrowing concern about the energy crisis and the seriousness of environmental contamination urgently demand the development of renewable energy sources as feasible alternatives to diminishing fossil fuels. Owing to its high energy density and environmentally friendly characteristics, molecular hydrogen is an attractive and promising energy carrier to meet future global energy demands1,2. In many of the approaches to hydrogen production, the electrocatalytic hydrogen evolution reaction (HER) from water splitting is the most economical and effective route for the future hydrogen economy3,4,5,6. To accelerate the sluggish HER kinetics, particularly in alkaline electrolytes, highly active and durable electrocatalysts are essential to lower the kinetic HER overpotential7,8. As a benchmark HER electrocatalyst with a zero HER overpotential, the precious metal platinum (Pt) plays a dominant role in present H2-production technologies, such as water-alkali electrolysers9,10,11. Unfortunately, the scarcity and high cost of Pt seriously impede its large-scale applications in electrocatalytic HERs.To develop efficient and earth-abundant alternatives to Pt as HER electrocatalysts, great efforts have been made to understand the fundamental HER mechanisms on the surfaces of electrocatalysts in alkaline environments12,13. The HER kinetics in alkaline solutions involves two steps: electron-coupled water dissociation (the Volmer step for the formation of adsorbed hydrogen); and the concomitant combination of adsorbed hydrogen into molecular hydrogen (the Heyrovsky or Tafel step; Supplementary Note 1)12,14. Accordingly, the HER activity of an electrocatalyst in alkaline electrolytes is synergistically dominated by the prior Volmer step and subsequent Tafel step13. The low energy barrier (ΔG(H2O)=0.44 eV) of the Volmer step provides the Pt catalyst with a fast Tafel step-determined HER process (Tafel slop=30 mV per decade) in alkaline electrolytes, which is responsible for its excellent HER activity12,15. Inspired by the fundamental HER mechanism that occurs on Pt, the development of novel Pt-free electrocatalysts with a significantly accelerated Volmer step is an appealing approach. Recently, several electrocatalysts with a decreased HER overpotential, such as CoP/S (with an overpotential at 10 mA cm−2: ∼48 mV) and Mo2C/graphene (with an overpotential at 10 mA cm−2: ∼34 mV) have been reported in acidic solutions16,17. Nevertheless, under alkaline conditions, the sluggish Volmer step on these Pt-free electrocatalysts results in far lower HER activity than the Pt catalyst18,19,20,21.In past decades, various Ni- or Mo-based oxides, hydroxides, layered double hydroxides, phosphides and sulfides have been reported as electrocatalysts for water splitting. Ni atoms are broadly recognized as excellent water dissociation centres, while Mo atoms have superior adsorption properties towards hydrogen13,22,23,24. Therefore, Mo–Ni-based alloy electrocatalysts (MoxNiy) can be promising candidates to effectively reduce the energy barrier of the Volmer step and speed up the sluggish HER kinetics under alkaline conditions. In this study, we demonstrate a MoNi4 electrocatalyst anchored on MoO2 cuboids, which are vertically aligned on nickel foam (MoNi4/MoO2@Ni). MoNi4 nanoparticles with a size of 20–100 nm are constructed in situ on the MoO2 cuboids by controlling the outward diffusion of Ni atoms when previously synthesized NiMoO4 cuboids are heated in a H2/Ar (v/v, 5/95) atmosphere at 500 °C. The resultant MoNi4/MoO2@Ni exhibits a high HER activity with a zero onset overpotential and a low Tafel slope of ∼30 mV per decade in a 1 M KOH aqueous solution, which are highly comparable to those for the Pt catalyst (onset overpotential: 0 mV; Tafel slope: 32 mV per decade). In addition, the achieved MoNi4 electrocatalyst requires low overpotentials of only ∼15 and ∼44 mV to stably deliver cathodic current densities of 10 and 200 mA cm−2, respectively, presenting state-of-the-art HER activity amongst all reported Pt-free electrocatalysts7,10,18. Experimental investigations reveal that the MoNi4 electrocatalyst behaves as the highly active centre and manifests fast Tafel step-determined HER kinetics. Furthermore, density functional theory (DFT) calculations determine that the kinetic energy barrier of the Volmer step for the MoNi4 electrocatalyst is as low as 0.39 eV. These results confirm that the sluggish Volmer step is drastically accelerated for the MoNi4 electrocatalyst.ResultsSynthesis of the MoNi4 electrocatalystThe synthesis of the MoNi4 electrocatalyst involves two steps, as illustrated in Fig. 1. First, the NiMoO4 cuboids were grown beforehand on a piece of nickel foam (1 × 3 cm2) via a hydrothermal reaction at 150 °C for 6 h in 15 ml of deionized water containing Ni(NO3)2·6H2O (0.04 M) and (NH4)6Mo7O24·4H2O (0.01 M). Second, when the as-synthesized NiMoO4 cuboids were calcined in a H2/Ar (v/v, 5/95) atmosphere at 500 °C for 2 h, the inner Ni atoms diffused outward due to the formation of MoO2. As a result, MoNi4 nanoparticles were directly constructed on the surfaces of the MoO2 cuboids. To probe the formation mechanism of the MoNi4 nanoparticles, different calcination temperatures and times were investigated (Supplementary Figs 1–5). In comparison with the smooth surfaces of precursor NiMoO4 at 400 °C, the appearance of numerous surface nanoparticles at 500 °C indicated the formation of MoNi4 on the resulting MoO2 cuboids (Supplementary Fig. 1a,b). When the calcination temperature reached 600 °C, MoNi3 nanoparticles on the MoO2 cuboids (MoNi3/MoO2@Ni) were produced due to the continuous reduction of MoO2 (Supplementary Fig. 1c,d). In addition, with increased calcination time at 500 °C, the MoNi4 nanoparticles gradually emerged and grew into bulk particles on the MoO2 cuboids (Supplementary Figs 2–5).Figure 1: Synthetic scheme of MoNi4 electrocatalyst supported by the MoO2 cuboids on nickel foam.Synthetic scheme of MoNi4 electrocatalyst supported by the MoO2 cuboids on nickel foam. Scale bars, Ni foam, 20 μm (top) and 1 μm (bottom); NiMoO4/Ni foam, 10 μm (top) and 2 μm (bottom); MoNi4/MoO2/Ni foam, 20 μm (top) and 1 μm (bottom).Full size imageStructural characterizations of the MoNi4 electrocatalystX-ray diffraction characterization reveals that the crystalline structure of the as-obtained precursor on the Ni foam can be indexed to NiMoO4 (Supplementary Fig. 6). The morphology of NiMoO4 was scrutinized by scanning electron microscopy (SEM). As shown in Supplementary Figs 7 and 8, dense NiMoO4 cuboids with sizes in the range of 0.5–1.0 μm and lengths of tens of microns are vertically aligned on the nickel foam. Elemental mapping, energy dispersive spectroscopy and X-ray photoelectron spectroscopy (XPS) confirm that the NiMoO4 cuboids consist of Ni, Mo and O elements, and the molar ratio of Ni to Mo is ∼1:1.01 (Supplementary Figs 9 and 10).The product of the NiMoO4 cuboids on the Ni foam calcined at 500 °C for 2 h was surveyed with X-ray diffraction using Cu-Kα radiation, SEM and high-resolution transmission electron microscopy (HRTEM). In Supplementary Fig. 11, the sharp X-ray diffraction diffraction peaks at ∼44.6°, 52.0° and 76.5° originate from the Ni foam (JCPDS, No. 65–2865). The peaks located at 26.3°, 37.0°, 41.5°, 49.5°, 53.7°, 60.5° and 66.9° are indexed to metallic MoO2 (JCPDS, No. 32-0671). The appearance of peaks at 31.0° and 43.5° are assigned to the (200) and (121) facets of MoNi4 (JCPDS, No. 65–5480), respectively. Thus, these result suggest that the obtained product on the nickel foam consists of MoNi4 and MoO2. As shown in Fig. 2a–c, numerous nanoparticles with sizes in the range of 20–100 nm are uniformly anchored on the cuboids, which are vertically aligned on the nickel foam. The corresponding energy-dispersive X-ray spectroscopy (EDX) analysis further confirms that the products are composed of Mo, Ni and O, and the molar ratio of Mo to Ni is ∼1:1.3 (Supplementary Fig. 12). Clearly, the HRTEM images of the samples show lattice fringes with lattice distances of 0.35 and 0.28 nm, which correspond to the (110) facet of MoO2 and the (200) facet of MoNi4, respectively (Fig. 2d–f). The selected-area electron diffraction pattern shows diffraction patterns of the (200) facet of MoNi4 and the (110) facet of MoO2 (the inset in Fig. 2d). Noticeably, the scanning TEM–EDX characterizations indicate that the surface nanoparticles are constituted by only Mo and Ni with an atomic ratio of 1:3.84, which well approaches to 1:4 (Fig. 2g and Supplementary Fig. 13). The XPS analysis was carried out to probe the chemical compositions and surface valence states of the MoNi4 nanoparticles and the supporting MoO2 cuboids. As illustrated in Supplementary Fig. 14, the XPS spectrum confirms the presence of Mo, Ni and O, and the molar ratio of Mo to Ni is ∼1:1.1. As shown in Supplementary Figs 15–17, XPS peaks of metallic Mo0 and Ni0 are observed at 229.3 and 852.5 eV, respectively, further confirming the existence of Mo0 and Ni0 in the surfaces of MoNi4/MoO2@Ni.Figure 2: Morphology and chemical composition analyses of MoNi4/MoO2@Ni.(a–c) Typical SEM and (d–f) HRTEM images of MoNi4/MoO2@Ni; (g) corresponding elemental mapping images of the MoNi4 electrocatalyst and the MoO2 cuboids. The inset image in d is the related selected-area electron diffraction pattern of the MoNi4 electrocatalyst and the MoO2 cuboids. Scale bars, (a) 20 μm; (b) 1 μm; (c) 100 nm; (d–f) 2 nm; inset in d, 1 1/nm; (g) 20 nm.Full size imageElectrocatalytic HER performanceTo evaluate the electrocatalytic HER activities of the electrocatalysts, a three-electrode system in an Ar-saturated 1 M KOH aqueous solution was used using a Hg/HgO electrode and a graphite rod as the reference and counter electrodes, respectively (Supplementary Fig. 18). All potentials are referenced to the reversible hydrogen electrode (RHE), and the ohmic potential drop loss from the electrolyte resistance has been subtracted (Supplementary Figs 19 and 20). For comparison, pure Ni nanosheets and MoO2 cuboids were also prepared on the nickel foam using the hydrothermal reactions (Supplementary Figs 21–25). As displayed in Fig. 3a and Supplementary Fig. 26, a commercial Pt/C electrocatalyst deposited on the nickel foam (weight density: 1 mg cm−2) using Nafion as a binder exhibited a zero HER onset overpotential and delivered a current density of 10 mV cm−2 at an overpotential of ∼10 mV. However, the maximum current density only reached 80 mA cm−2 due to the Pt catalyst significantly peeling off from the support, caused by the generated H2 bubbles. Although the Ni nanosheets on the nickel foam could act as an HER electrocatalyst, the HER occurred at a very high overpotential of ∼253 mV. For the MoO2 cuboids on the nickel foam, the cathodic current density of 10 mA cm−2 was delivered at an overpotential as large as ∼48 mV. In comparison to the Ni nanosheets and the MoO2 cuboids, the NiMoO4 cuboids and MoNi3/MoO2 cuboids on the nickel foam exhibited a similar onset overpotential of ∼10 mV and an overpotential of ∼30 and 37 mV at 10 mA cm−2, respectively (Supplementary Figs 27–29). Remarkably, MoNi4/MoO2@Ni exhibited an onset overpotential of 0 mV, which was highly comparable to that of the Pt catalyst. In addition, for the supported MoNi4 electrocatalyst, the overpotential at current densities of 10 and 200 mA cm−2 was as low as ∼15 and 44 mV, respectively, which were significantly lower than the values for the Ni nanosheets, MoO2 cuboids, NiMoO4 cuboids, MoNi3/MoO2 cuboids and state-of-the-art Pt-free HER electrocatalysts such as NiO/Ni heterostructures (∼85 mV at 10 mA cm−2)25, pyrite-type CoPS nanowires (∼48 mV at 10 mA cm−2)16, nickel doped carbon (∼34 mV at 10 mA cm−2)26, a Mo2C/carbon/graphene hybrid (∼34 mV at 10 mA cm−2)17, MoSSe/NiSe2 foam (∼69 mV at 10 mA cm−2)27, Fe0.9Co0.1S2/carbon nanotubes (∼100 mV at 10 mA cm−2)28, Ni2P nanoparticles (∼120 mV at 10 mA cm−2)29 and strained MoS2 nanosheets (∼170 mV at 10 mA cm−2)30 (Supplementary Table 1)31,32,33,34,35,36,37,38,39.Figure 3: Electrocatalytic activities of different catalysts.(a) Polarization curves and (b) Tafel plots of the MoNi4 electrocatalyst supported by the MoO2 cuboids, pure Ni nanosheets and MoO2 cuboids on the nickel foam. (c) Comparison with selected state-of-the-art HER electrocatalysts. (d) Polarization curves of the MoNi4 electrocatalyst before and after 2,000 cyclic voltammetry cycles; inset: long-term stability tests of the MoNi4 electrocatalyst at different current densities: 10; 100; and 200 mA cm−2. Electrolyte: 1 M KOH aqueous solution; scan rate: 1 mV s−1.Full size imageFigure 3b displays the Tafel plots of the corresponding polarization curves, which provide profound insights into the fundamental HER kinetic mechanism occurring on the surfaces of the electrocatalysts. As a result of the low energy barrier (0.44 eV on Pt) of the Volmer step, the kinetic rate-limiting step for the Pt catalyst is the Tafel process, and the theoretical Tafel slope is 30 mV per decade (here the Tafel slope of the commercial Pt catalyst was measured to be 32 mV per decade)12. Remarkably, the Tafel slope of the MoNi4 electrocatalyst was as low as 30 mV per decade, which is far lower than the values of 129 mV per decade for the Ni nanosheets and 75 mV per decade for the MoO2 cuboids and highly comparable to that of the Pt-based catalyst (Fig. 3c and Supplementary Table 1). This result indicated that the electrocatalytic HER kinetics on the MoNi4 electrocatalyst were determined by the Tafel step rather than a coupled Volmer–Tafel or Volmer–Heyrovsky process. In other words, the prior Volmer step has been significantly accelerated. The exchange current density of the MoNi4 electrocatalyst was estimated to be ∼1.24 mA cm−2 (Supplementary Fig. 30). To clarify the influence of the active surface area on the electrocatalytic HER activity, the corresponding electrochemical double-layer capacitances (Cps) of the electrocatalysts were analysed by applying cyclic voltammetry cycles at different scan rates40. The Cps of the Ni nanosheets and MoO2 cuboids were ∼0.001 and 0.640 F, respectively, while the MoNi4 electrocatalyst had a high Cp of 2.220 F (Supplementary Fig. 31). On the basis of its Cp, the MoNi4 electrocatalyst was calculated to have a turnover frequency of 0.4 s−1 at a low overpotential of 50 mV, which was higher than the turnover frequency values of the previously reported Pt-free electrocatalysts (Supplementary Fig. 32 and Supplementary Table 1)41,42,43,44.Long-term electrocatalytic stability is another important criterion for HER electrocatalysts. To investigate the durability of the MoNi4 electrocatalyst, continuous cyclic voltammetry scans were performed between 0.2 and −0.2 V at a scan rate of 50 mV s−1 in a 1 M KOH solution. As depicted in Fig. 3d, the HER overpotential of the MoNi4 electrocatalyst at 200 mA cm−2 increased by only 6 mV after 2,000 cyclic voltammetry cycles. In addition, a long-term electrocatalytic HER process was successively carried out at current densities of 10, 100 and 200 mA cm−2 (Supplementary Movie 1). The inset in Fig. 3d demonstrates that the MoNi4 electrocatalyst retained a steady HER activity, and only an increase of ∼3 mV in potential was observed at a current density of 10 mA cm−2 after a period of 10 h of hydrogen production. The overpotential required for large current densities of 100 and 200 mA cm−2 was augmented by only 2 and 5 mV, respectively. After a series of HER durability assessments, the structure of the MoNi4 electrocatalyst was examined using SEM and HRTEM. MoNi4/MoO2@Ni showed no structural variations, highlighting the superior structural robustness of the MoNi4 electrocatalyst during the electrocatalytic HER process (Supplementary Figs 33–36).The approach to the synthesis of MoNi4/MoO2@Ni is scalable on the nickel foam. The MoNi4 electrocatalyst was thus prepared on commercially available nickel foam with dimensions of 6 × 20 cm2. As shown in Supplementary Fig. 37, the MoNi4 electrocatalyst supported by the MoO2 cuboids on the nickel foam was free-standing and highly flexible. It is notable that the MoNi4 electrocatalyst unveiled a steady HER activity even though the supporting Ni foam was deformed to various degrees (Supplementary Fig. 38). For reported Raney nickel and nickel–molybdenum alloy electrodes, concentrated alkaline solutions (30 wt%) and high electrolyte temperatures (70 °C) are generally demanded to achieve high cathodic current densities of 200–500 mA cm−2 (ref. 45). Here high cathodic current densities of up to 200 and 500 mA cm−2 were delivered by the MoNi4 electrocatalyst at extremely low overpotentials of ∼44 and ∼65 mV in a 5.3 wt% KOH solution at room temperature.Afterward, a water-alkali electrolyser was built up in a 1 M KOH solution using MoNi4/MoO2@Ni as the cathode and a previously reported MoS2/Ni3S2 hybrid as the anode (Supplementary Fig. 39)38. As exhibited in Supplementary Fig. 40a, for a noble metal-based Pt–Ir/C couple, a cell voltage of ∼1.7 V was applied for a current density of 10 mA cm−2. In contrast, the MoNi4–MoS2/Ni3S2 couple required a low cell voltage of only ∼1.47 V to deliver a current density of 10 mA cm−2, which is much lower than that for the noble metal-based Pt–Ir/C couple. Over 10 h of galvanostatic electrolysis at 10 mA cm−2, the applied voltage of the MoNi4–MoS2/Ni3S2 couple had an augmentation of ∼0.02 V, which is much lower than the value of 0.07 V for the Pt–Ir/C couple (Supplementary Fig. 40b). Moreover, the electrolyser with a high current density of 200 mA cm−2 was durably driven by the MoNi4–MoS2/Ni3S2 couple at a low voltage of ∼1.70 V (Supplementary Movie 2).HER active centresTo understand the intrinsic contributions of the surface MoNi4 nanoparticles and the underlying MoO2 cuboids to the HER activity, pure MoO2 nanosheets and MoNi4 nanoparticles supported by MoO2 cuboids were also synthesized on carbon cloth. Thus, the contribution of the underlying Ni foam could be excluded (Supplementary Fig. 41). Clearly, the pristine MoO2 nanosheets on carbon cloth showed a very high HER onset potential of ∼240 mV in 1 M KOH and ∼200 mV in 0.5 M H2SO4, suggesting that the MoO2 electrocatalyst inherently presented a very sluggish Volmer step and a poor Tafel process (Supplementary Fig. 42). In contrast, the MoNi4 electrocatalyst supported by the MoO2 cuboids on the carbon cloth (MoNi4/MoO2@C) exhibited a zero onset potential, which was similar to that for MoNi4/MoO2@Ni. When the surface MoNi4 nanoparticles of MoNi4/MoO2@C were etched away using 2 M H2SO4 aqueous solution. Obviously, the produced MoO2@C showed a largely increased onset potential of ∼133 mV (Supplementary Figs 43–46). These results demonstrate that the excellent HER activity of the MoNi4/MoO2@Ni unambiguously originates from the surface MoNi4 nanoparticles rather than from the supporting MoO2 cuboids.To gain profound insight into the electrocatalytic HER active sites, we also analysed the surface electrochemical behaviour of the MoNi4 electrocatalyst on the MoO2 cuboids. For a freshly prepared MoNi4 electrocatalyst, an electrochemical cyclic voltammetry cycle between −0.025 and 0.275 V (versus RHE) was initially performed with a scan rate of 1 mV s−1. Obviously, the positions of the electrochemically reversible peaks shifted from 0.175 V/0.113 V to 0.215 V/0.064 V when the KOH concentration was changed from 1 to 0.1 M (Supplementary Fig. 47a). The strong dependence on the concentration of KOH as the electrolyte revealed that the electrochemically reversible peaks originated from an ad-/desorption process of water molecules or hydrogen (between 0.05 and 0.35 V, as reported) rather than from the surface redox reactions of the MoNi4 electrocatalyst and supporting MoO2 cuboids12. In addition, in contrast to the results on pure Ni nanosheets (0.150 V) and MoO2 (0.164 V) cuboids, the water or hydrogen adsorption peak of the MoNi4 electrocatalyst showed an anodic shift to 0.175 V, reflecting a superior water or hydrogen adsorption property (Supplementary Fig. 47b).To evaluate the intrinsic electrocatalytic HER activity of the MoNi4 electrocatalyst, the recorded cathodic current density was normalized versus the related Brunauer Emmett Teller specific surface area of the MoNi4 electrocatalyst (32 m2 g−1) (Supplementary Fig. 48). As described in Supplementary Fig. 49, when the current density was below 0.38 A m−2, the polarization curve of the MoNi4 electrocatalyst nearly overlapped with that of the Pt catalyst. However, the HER overpotential of the MoNi4 electrocatalyst was much lower than that of the Pt catalyst at large current densities (>0.38 A m−2). These results illustrate that the intrinsic HER activity associated with the specific surface area of the MoNi4 electrocatalyst is even higher than that of the Pt catalyst under alkaline conditions.Theoretical calculationsTo understand the fundamental mechanism of the outstanding HER activity on MoNi4/MoO2@Ni, the kinetic energy barrier of the prior Volmer step (ΔG(H2O)) and the concomitant combination of adsorbed H into molecular hydrogen (ΔG(H), Tafel step) were studied using the DFT calculations according to the as-built electrocatalyst models including the (111) facet of Ni metal, the (110) facet of Mo metal, the (110) facet of MoO2 and the (200) facet of MoNi4 (Supplementary Fig. 50). As shown in Fig. 4, MoO2 has a large energy barrier for the Volmer step (ΔG(H2O)=1.01 eV) and a strong hydrogen adsorption free energy (|ΔG(H)|=1.21 eV), indicating a very sluggish Volmer–Tafel mechanism. Thus, MoO2 is not the highly active centre for the HER, which agrees well with the experimental results. The ΔG(H2O) values on pure Ni metal and Mo metal are as high as 0.91 and 0.65 eV, respectively (Fig. 4b and Supplementary Fig. 51). In contrast, the ΔG(H2O) on MoNi4 is significantly decreased to 0.39 eV, which is even lower than the value of 0.44 eV on Pt (ref. 15). In addition, MoNi4 has a lower |ΔG(H)| of 0.74 eV than the value of 1.21 eV for MoO2, which corresponds to a superior hydrogen adsorption capability (Fig. 4c). Thereby, the HER reaction on MoNi4 is associated with a process defined by a fast Tafel step rather than a sluggish Volmer–Tafel step (Supplementary Fig. 52).Figure 4: DFT calculations.(a) Calculated free energies of H2O adsorption, activated H2O adsorption, OH adsorption and H adsorption. (b) Calculated adsorption free energy diagram for the Volmer step. (c) Calculated adsorption free energy diagram for the Tafel step. Blue balls: Ni; aqua balls: Mo; red balls: O.Full size imageDiscussionIn summary, we have demonstrated a MoNi4 electrocatalyst supported by MoO2 cuboids on nickel foam or carbon cloth. As favoured by a largely reduced energy barrier of the Volmer step, the achieved MoNi4 electrocatalyst exhibits a high HER activity under alkaline conditions, which is highly comparable to that for Pt and outperforms any reported results for Pt-free electrocatalysts, to the best of our knowledge. Moreover, the large-scale preparation and excellent catalytic stability provide MoNi4/MoO2@Ni with a promising utilization in water-alkali electrolysers for hydrogen production. Therefore, the exploration and understanding of the MoNi4 electrocatalyst provide a promising alternative to Pt catalysts for emerging applications in energy generation.MethodsMaterial synthesisTo synthesize the MoNi4 electrocatalyst, NiMoO4 cuboids were first constructed on nickel foam through a hydrothermal reaction46. First, the commercial nickel foam was successively washed with ethanol, a 1 M HCl aqueous solution and deionized water. Second, one piece of nickel foam (1 × 3 cm2) was immersed into 15 ml of H2O containing Ni(NO3)2·6H2O (0.04 M) and (NH4)6Mo7O24·4H2O (0.01 M) in a Teflon autoclave. Third, the autoclave was heated at 150 °C for 6 h in a drying oven. After washing with deionized water, the NiMoO4 cuboids were achieved on the nickel foam. Finally, the as-constructed NiMoO4 cuboids were heated at 500 °C for 2 h in a H2/Ar (4:96) atmosphere, and then, the MoNi4 electrocatalyst anchored on the MoO2 cuboids was obtained. The loading weight of the formed MoNi4 nanoparticles and MoO2 cuboids on the nickel foam was ∼43.4 mg cm2. The pure Ni nanosheets and MoO2 cuboids on the nickel foam, as well as the pure MoO2 nanosheets and MoN4 nanoparticles supported by MoO2 cuboids on carbon cloth, were also prepared following the same procedure for MoNi4 by changing the precursors and substrates.Structure characterizationsSEM, as well as corresponding elemental mapping, and EDX analysis were carried out with a Gemini 500 (Carl Zeiss) system. HRTEM was performed using a LIBRA 200 MC Cs scanning TEM (Carl Zeiss) operating at an accelerating voltage of 200 kV. XPS experiments were carried out on an AXIS Ultra DLD (Kratos) system using Al Kα radiation. XRD patterns were recorded on a PW1820 powder diffractometer (Phillips) using Cu-Kα radiation. The electrochemical tests were carried out on WaveDriver 20 (Pine Research Instrumentation) and CHI 660E Potentiostat (CH Instruments) systems.Electrochemical measurementsAll electrochemical tests were performed at room temperature. The electrochemical HER was carried out in a three-electrode system. A standard Hg/HgO electrode and a graphite rod were used as the reference and counter electrodes, respectively. The Hg/HgO electrode was calibrated using bubbling H2 gas on a Pt coil electrode. Potentials were referenced to an RHE by adding 0.923 V (0.099+0.059 × pH) in a 1 M KOH aqueous solution. For comparison, Pt/C (20 wt%, FuelCellStore; loaded on the nickel foam at 1 mg cm−2) was used as an HER electrocatalyst. The impedance spectra of the electrocatalysts in a three-electrode set-up were recorded at different HER overpotentials in a 1 M KOH electrolyte. All voltages and potentials were corrected to eliminate electrolyte resistances unless noted. Electrolyte resistance: 0.94 Ω; scan rate: 1 mV s−1.Theoretical calculationsAll computations were performed by applying the plane-wave-based DFT method with the Vienna Ab Initio Simulation Package and periodic slab models. The electron ion interaction was described with the projector augmented wave method. The electron exchange and correlation energy were treated within the generalized gradient approximation in the Perdew–Burke–Ernzerhof formalism. The cut-off energy of 400 eV and Gaussian electron smearing method with σ=0.05 eV were used. The geometry optimization was performed when the convergence criterion on forces became smaller than 0.02 eV Å−1 and the energy difference was <10−4 eV. The adsorption energy (Eads) of species X is calculated by Eads=E(X/slab)−E(X)−E(slab), and a more negative Eads indicates a more stable adsorption. For the DFT calculations, the reactant (H2O) and intermediates (OH and H) are first adsorbed on all possible active sites of the catalyst. Afterwards, the VASP software is utilized to optimize the adsorption. For evaluating the energy barrier (Ea=ETS−EIS), the transitional state (TS) was located using the Nudged Elastic Band method. All transition states were verified by vibration analyses with only one imaginary frequency. The p(3 × 3)-Ni(111), p(3 × 3)-Mo(110), p(3 × 3)-MoO2(110) and p(1 × 1)-MoNi4(200) surfaces were utilized to simulate the properties of these electrocatalysts.Data availabilityThe data that support the findings of this study are available from the corresponding author on reasonable request.Additional informationHow to cite this article: Zhang, J. et al. Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics. Nat. Commun. 8, 15437 doi: 10.1038/ncomms15437 (2017).Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

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Download referencesAcknowledgementsThis work was financially supported by the ERC Grant on 2DMATER and EC under Graphene Flagship (No. CNECT-ICT-604391). We also acknowledge the Cfaed (Center for Advancing Electronics Dresden), the Dresden Center for Nanoanalysis (DCN) at TU Dresden and Dr Horst Borrmann for the X-ray diffraction characterizations in Max Planck Institute for Chemical Physics of Solids.Author informationAuthors and AffiliationsCenter for Advancing Electronics Dresden (Cfaed) and Department of Chemistry and Food Chemistry, Technische Universitaet Dresden, Dresden, 01062, GermanyJian Zhang, Shaohua Liu, Xiaodong Zhuang & Xinliang FengUniv Lyon, Ens de Lyon, CNRS, Université Lyon 1, Laboratoire de Chimie, UMR 5182, Lyon, F-69342, FranceTao WangWPI Advanced Institute for Materials Research, Tohoku University, Sendai, 980-8577, JapanPan Liu & Mingwei ChenCREST, JST, 4-1-8 Honcho Kawaguchi, Saitama, 332-0012, JapanPan Liu & Mingwei ChenFraunhofer Institute for Ceramic Technologies and Systems (IKTS), Dresden, 01109, GermanyZhongquan Liao & Ehrenfried ZschechAuthorsJian ZhangView author publicationsYou can also search for this author in

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PubMed Google ScholarContributionsJ.Z. and X.F. conceived and designed the experiments and wrote the paper; J.Z. carried out the synthesis and characterization of electrocatalysts; T.W. performed the DFT calculations; P.L., S.L., Z.L., X.Z., M.C. and E.Z. assisted with the HRTEM and XPS characterizations. All authors discussed the results and commented on the manuscript.Corresponding authorCorrespondence to

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Supplementary informationSupplementary InformationSupplementary Figures, Supplementary Table, Supplementary Note and Supplementary References (PDF 5343 kb)Supplementary Movie 1Electrocatalytic hydrogen evolution in a three-electrode cell. (MOV 8511 kb)Supplementary Movie 2Alkaline water splitting electrolyzer. (MOV 8618 kb)Peer Review File (PDF 1131 kb)Rights and permissions

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Reprints and permissionsAbout this articleCite this articleZhang, J., Wang, T., Liu, P. et al. Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics.

Nat Commun 8, 15437 (2017). https://doi.org/10.1038/ncomms15437Download citationReceived: 28 November 2016Accepted: 30 March 2017Published: 17 May 2017DOI: https://doi.org/10.1038/ncomms15437Share this articleAnyone you share the following link with will be able to read this content:Get shareable linkSorry, a shareable link is not currently available for this article.Copy to clipboard

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将 MoO4 四面体活化为 MoNi 合金中的 MoOx 物种，以提高碱性析氢反应的性能,Chemical Engineering Journal - X-MOL

将 MoO4 四面体活化为 MoNi 合金中的 MoOx 物种，以提高碱性析氢反应的性能,Chemical Engineering Journal - X-MOL

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将 MoO4 四面体活化为 MoNi 合金中的 MoOx 物种，以提高碱性析氢反应的性能

Chemical Engineering Journal

(

IF

15.1

)

Pub Date : 2023-06-09

, DOI:

10.1016/j.cej.2023.143846

Zhengyuan Zhang, Longhua Li, Yihuan Li, Yiyang Zheng, Qian Wu, Lijuan Xie, Bifu Luo, Jinhui Hao, Weidong Shi

MoNi 合金作为优异的碱性析氢反应 (HER) 电催化剂受益于活化的 Mo 基聚合物以优化 Ni 位点的氢解吸。Mo基聚合物由吸附的MoO 4 2-转化而成，MoO 4 2- 由溶解的Mo形成。然而，Mo的溶解行为是不可控的，吸附的MoO 4 2-是有限的，导致MoNi合金的活性降低。在此，我们报道了一种晶胞活化策略，用于在 MoNi (MoO x /MoNi) 合金中制备活化的 MoO x物种，以提高碱性 HER 的性能。拉曼光谱表征表明，MoNi合金中活化的MoO x物种主要来源于MoO 4HER下β-NiMoO 4的四面体结构与催化剂的HER性能有很强的相关性。获得的 MoO x /MoNi 具有出色的 HER 活性，具有低过电位和 Tafel 斜率，分别为 35 mV@10 mA cm -2和 58 mV dec -1，甚至超过商业 Pt/C。正如一系列表征技术和理论方法所揭示的那样，出色的 HER 活性可归因于 MoOx 调节 Ni 位点氢解吸的能力和MoNi 合金的本征性质。重要的是，将 MoO 4四面体激活为 MoO x物种是取代Mo在MoNi合金中自溶重构的有效途径，可以有效减少溶解的Mo对MoNi合金催化活性的不利影响。这项工作展示了 MoO 4四面体到 MoO x物种的活化过程，为通过晶胞活化而不是自溶解和重组来设计和制造高性能 HER 催化剂提供了新的见解。

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Activating MoO4 tetrahedrons to MoOx species in MoNi alloy for boosting performance in alkaline hydrogen evolution reaction

MoNi alloys as excellent alkaline hydrogen evolution reaction (HER) electrocatalysts benefit from activated Mo-based polymerides for optimizing hydrogen desorption of Ni site. Mo-based polymerides are transformed from adsorbed MoO42−, which is formed by dissolved Mo. However, the dissolution behavior of Mo is uncontrollable and adsorbed MoO42− is limited, resulting in reduced activity of the MoNi alloys. Herein, we reported a unit cell activation strategy to prepare activated MoOx species in MoNi (MoOx/MoNi) alloy for boosting performance in alkaline HER. Characterization by Raman spectroscopy shows that activated MoOx species in MoNi alloy are mainly derived from MoO4 tetrahedrons of the β-NiMoO4 under HER, which have strong correlation with the HER performance of the catalyst. The obtained MoOx/MoNi performs a brilliant HER activity with a low overpotential and Tafel slope of 35 mV@10 mA cm−2 and 58 mV dec−1, respectively, even surpassing commercial Pt/C. As revealed by a series of characterization techniques and theoretical methods, the brilliant HER activity can be ascribed to both the capacity of MoOx on adjusting the hydrogen desorption of Ni site and the intrinsic property of the MoNi alloy. Significantly, activating MoO4 tetrahedrons to MoOx species is an efficient way to replace the self-dissolution and restructure of Mo in MoNi alloy, which could effectively minimize the adverse effect of dissolved Mo on the catalytic activity of MoNi alloy. This work demonstrates the activation process of MoO4 tetrahedrons to MoOx species, providing a new insight into designing and fabricating high-performance HER catalysts by unit cell activation instead of self-dissolution and restructure.

更新日期：2023-06-10

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