Sulfophobic and Vacancy Design Enables Self-Cleaning Electrodes for Efficient Desulfurization and Concurrent Hydrogen Evolution with Low Energy Consumption

Zhang Shuo; Zhou Qingwen; Shen Zihan; Jin Xin; Zhang Yuchen; Shi Man; Zhou Jian; Liu Jianguo; Lu Zhenda; Zhou Yong-Ning; Zhang Huigang

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Sulfophobic and Vacancy Design Enables Self-Cleaning Electrodes for Efficient Desulfurization and Concurrent Hydrogen Evolution with Low Energy Consumption

机译：硫虫和空位设计使自清洁电极能够有效脱硫和氢气进化的低能量消耗

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Sulfide oxidation reaction (SOR) is one central step of electrochemical desulfurization and sulfur-based batteries. However, the electrochemical performance of desulfurization and sulfur batteries has been severely hindered by sulfur passivation. Here, a discovery of sulfophobic phenomenon of electrocatalysts having weak interaction to sulfur species is reported. A self-cleaning NiS2 electrode is developed to avoid the long-perplexing passivation issue of solid sulfur during the SOR. Furthermore, sulfur-vacancies are engineered into NiS2 lattice to synthesize v-NiS2 for the hydrogen evolution reaction (HER). The resultant lattice expansion and electron redistribution can adjust the adsorbed hydrogen to reach a nearly thermos-neutral state, enabling high catalytic activity for the HER. By coupling the HER and SOR, efficient desulfurization and simultaneous hydrogen production is demonstrated. Bifunctional NiS2 enables such a one-stone-kills-two-birds strategy to realize continuous electrochemical desulfurization with superior energy efficiency (1.05 g(sulfur) Wh(-1)). As a general design principle, sulfophobic electrocatalysts can improve the properties of lithium-sulfur batteries by minimizing the passivation of S-8 during charge. In brief, interfacial interaction between electrocatalysts and sulfur species are systematically investigated and a sulfophobic strategy to significantly enhance the electrochemical performance of the SOR is offered.

机译：硫化物氧化反应（SOR）是电化学脱硫和硫基电池的一种中央步骤。然而，通过硫钝化严重阻碍了脱硫和硫电池的电化学性能。这里，据报道，据报道了对具有弱相互作用的电催化剂对硫物质的硫杂交现象的发现。开发了一种自清洁NIS2电极以避免在SOR期间的固体硫的长杂交钝化问题。此外，硫 - 空位被设计成NIS2晶格以合成V-NIS2以用于氢进化反应（她）。所得晶格膨胀和电子再分配可以调节吸附的氢以达到几乎热循环状态，从而为她提供高催化活性。通过偶联她和SOR，证实了高效的脱硫和同时氢气产生。双功能NIS2使得这种单石杀死两只鸟策略能够实现具有卓越能效的连续电化学脱硫（1.05g（硫）WH（-1））。作为一般的设计原理，通过最小化电荷期间S-8的钝化可以改善锂 - 硫电池的性质。简而言之，系统地研究了电催化剂和硫种类之间的界面相互作用，并提供了硫化物策略，可显着提高SOR的电化学性能。

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来源
《Advanced Functional Materials》 |2021年第31期|2101922.1-2101922.11|共11页
作者
Zhang Shuo; Zhou Qingwen; Shen Zihan; Jin Xin; Zhang Yuchen; Shi Man; Zhou Jian; Liu Jianguo; Lu Zhenda; Zhou Yong-Ning; Zhang Huigang;
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Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China|Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China;

Nantong Univ Sch Publ Hlth Inst Environm Hlth & Green Chem Nantong Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China;

Fudan Univ Dept Mat Sci Shanghai 200433 Peoples R China;

Nanjing Univ Coll Engn & Appl Sci Natl Lab Solid State Microstruct Collaborat Innovat Ctr Adv Microstruct Nanjing 210093 Jiangsu Peoples R China|Nanjing Univ Inst Mat Engn Nanjing 210093 Jiangsu Peoples R China|Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China;

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正文语种 eng
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hydrogen evolution reaction; low energy consumption; nickel disulfide; self-cleaning electrodes; sulfide removal;

机译：氢进化反应;低能耗;镍二硫化物;自清洁电极;硫化物去除;

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2. Hydrogen Production: 3D Self‐Architectured Steam Electrode Enabled Efficient and Durable Hydrogen Production in a Proton‐Conducting Solid Oxide Electrolysis Cell at Temperatures Lower Than 600 °C (Adv. Sci. 11/2018) [J] . Wei Wu, Hanping Ding, Yunya Zhang, Advanced Science . 2018,第11期

机译：氢气产生：在低于600°C的温度下，质子传导固体氧化物电解池中的3D自构蒸汽电极可实现高效且持久的氢气产生（Adv.Sci.11 / 2018）
3. Facile and Efficient Atomic Hydrogenation Enabled Black TiO_2 with Enhanced Photo-Electrochemical Activity via a Favorably Low-Energy-Barrier Pathway [J] . Wang Xiaodan, Mayrhofer Leonhard, Hoefer Markus, Advanced energy materials . 2019,第33期

机译：通过有利的低能垒途径，实现了高效，高效的原子氢化，使黑色TiO_2具有增强的光电化学活性
4. Reactions at a Porous Ni electrode Concurrent with Hydrogen Evolution [C] . M Villa, P. Salvi, E. Verardi, Ionic and mixed conducting ceramics 6 . 2008

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5. Design and study of catalytic activators of hydrogen peroxide promising rapid, efficient petroleum desulfurization and bleaching technologies. [D] . Hangun, Yelda. 2002

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6. 3D Self‐Architectured Steam Electrode Enabled Efficient and Durable Hydrogen Production in a Proton‐Conducting Solid Oxide Electrolysis Cell at Temperatures Lower Than 600 °C [O] . Wei Wu, Hanping Ding, Yunya Zhang, 2018

机译：3D自构蒸汽电极可在质子传导性固体氧化物电解槽中在低于600°C的温度下高效且持久地产生氢气
7. 3D Self‐Architectured Steam Electrode Enabled Efficient and Durable Hydrogen Production in a Proton‐Conducting Solid Oxide Electrolysis Cell at Temperatures Lower Than 600 °C [O] . Wei Wu, Hanping Ding, Yunya Zhang, 2018

机译：3D自建筑蒸汽电极在温度低于600°C的温度下，在质子导电的固体氧化物电解槽中能够高效和耐用的氢气生产

Sulfophobic and Vacancy Design Enables Self-Cleaning Electrodes for Efficient Desulfurization and Concurrent Hydrogen Evolution with Low Energy Consumption

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