Ruthenium Nanoclusters and Single Atoms on α-MoC/N-Doped Carbon Achieves Low-Input/Input-Free Hydrogen Evolution via Decoupled/Coupled Hydrazine Oxidation

被引：22

作者：

Li, Yapeng ^{[1
,2
]}

Niu, Shuwen ^{[1
,3
]}

Liu, Peigen ^{[2
]}

Pan, Rongrong ^{[1
,2
]}

Zhang, Huaikun ^{[4
]}

Ahmad, Nazir ^{[4
]}

Shi, Yi ^{[2
]}

Liang, Xiao ^{[5
]}

Cheng, Mingyu ^{[4
]}

Chen, Shenghua ^{[5
]}

Du, Junyi ^{[6
]}

Hu, Maolin ^{[1
]}

Wang, Dingsheng ^{[5
]}

Chen, Wei ^{[1
]}

Li, Yadong ^{[5
]}

机构：

[1] Wenzhou Univ, Coll Chem & Mat Engn, Key Lab Carbon Mat Zhejiang Prov, Wenzhou 325035, Zhejiang, Peoples R China

[2] Univ Sci & Technol China, Ctr Adv Nanocatalysis CAN, Dept Appl Chem, Hefei 230026, Anhui, Peoples R China

[3] Qingdao Univ, Coll Chem & Chem Engn, Qingdao 266071, Shangdong, Peoples R China

[4] Univ Sci & Technol China, Dept Mat Sci & Engn, CAS Key Lab Mat Energy Convers, Hefei 230026, Anhui, Peoples R China

[5] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

[6] Chinese Acad Sci, Suzhou Inst Nanotech & Nanob, Key Lab Multifunct Nanomat & Smart Syst, Div Adv Mat, Suzhou 215123, Jiangsu, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2024年 / 63卷 / 30期

基金：

中国博士后科学基金; 中国国家自然科学基金;

关键词：

Ru single atoms; Ru nanoclusters; Hydrogen Evolution Reaction; Hydrazine Oxidation Reaction; Bifunctionality; METAL-ORGANIC FRAMEWORKS; WATER-GAS SHIFT; OXYGEN REDUCTION; PH-UNIVERSAL; EFFICIENT; NANOPARTICLES; RU; ELECTROCATALYSTS; PERFORMANCE; NANOWIRES;

D O I：

10.1002/anie.202316755

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The hydrazine oxidation-assisted H2 evolution method promises low-input and input-free hydrogen production. However, developing high-performance catalysts for hydrazine oxidation (HzOR) and hydrogen evolution (HER) is challenging. Here, we introduce a bifunctional electrocatalyst alpha-MoC/N-C/RuNSA, merging ruthenium (Ru) nanoclusters (NCs) and single atoms (SA) into cubic alpha-MoC nanoparticles-decorated N-doped carbon (alpha-MoC/N-C) nanowires, through electrodeposition. The composite showcases exceptional activity for both HzOR and HER, requiring -80 mV and -9 mV respectively to reach 10 mA cm-2. Theoretical and experimental insights confirm the importance of two Ru species for bifunctionality: NCs enhance the conductivity, and its coexistence with SA balances the H ad/desorption for HER and facilitates the initial dehydrogenation during the HzOR. In the overall hydrazine splitting (OHzS) system, alpha-MoC/N-C/RuNSA excels as both anode and cathode materials, achieving 10 mA cm-2 at just 64 mV. The zinc hydrazine (Zn-Hz) battery assembled with alpha-MoC/N-C/RuNSA cathode and Zn foil anode can exhibit 97.3 % energy efficiency, as well as temporary separation of hydrogen gas during the discharge process. Therefore, integrating Zn-Hz with OHzS system enables self-powered H2 evolution, even in hydrazine sewage. Overall, the amalgamation of NCs with SA achieves diverse catalytic activities for yielding multifold hydrogen gas through advanced cell-integrated-electrolyzer system. The synergistic activation of the bifunctional reaction kinetics of cubic alpha-MoC nanoparticles decorated-N-doped carbon by the concomitant Ru nanoclusters and single atom enables the efficient coupling or decoupling of hydrazine oxidation reaction and hydrogen evolution reaction for the multifold H2 production via the zinc hydrazine battery-driven overall hydrazine splitting system. image

引用

页数：13

共 2 条

[1] Ir nanoclusters/porous N-doped carbon as a bifunctional electrocatalyst for hydrogen evolution and hydrazine oxidation reactions
Huang, Hong-Li
Guan, Xiya
Li, Haibo
Li, Ruiqing
Li, Rui
Zeng, Suyuan
Tao, Shuo
Yao, Qingxia
Chen, Hongyan
Qu, Konggang
CHEMICAL COMMUNICATIONS, 2022, 58 (14) : 2347 - 2350
[2] Ru single atoms and nanoclusters on highly porous N-doped carbon as a hydrogen evolution catalyst in alkaline solutions with ultrahigh mass activity and turnover frequency
Li, Yijun
Liu, Huijing
Li, Bing
Yang, Zhenzhen
Guo, Zhenguo
He, Jian-Bo
Xie, Jianhui
Lau, Tai-Chu
JOURNAL OF MATERIALS CHEMISTRY A, 2021, 9 (20) : 12196 - 12202

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