Pt-Loaded CoFe-Layered Double Hydroxides for Simultaneously Driving HER and HzOR

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-09-25 DOI:10.1021/acscatal.4c03881

Tianrui Yu, Guihao Liu, Tianqi Nie, Zhaohui Wu, Ziheng Song, Xiaoliang Sun, Yu-Fei Song

{"title":"Pt-Loaded CoFe-Layered Double Hydroxides for Simultaneously Driving HER and HzOR","authors":"Tianrui Yu, Guihao Liu, Tianqi Nie, Zhaohui Wu, Ziheng Song, Xiaoliang Sun, Yu-Fei Song","doi":"10.1021/acscatal.4c03881","DOIUrl":null,"url":null,"abstract":"Hydrazine-assisted water electrolysis presents an energy-saving pathway for H2 production. However, due to the different electronic structure requirements for active metals in hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) reactions, catalysts capable of simultaneously driving HER and HzOR are less studied. Herein, we employ an electrochemical deposition method to load 4.2 nm Pt nanoparticles onto CoFe-layered double hydroxides. The resultant Pt/CoFe/NF requires only 12.1 and 28.7 mV to achieve 50 and 100 mA cm–2 for HzOR and an ultralow overpotential of 16.5 mV with a Tafel slope of 31.4 mV dec–1 to achieve 10 mA cm–2 for HER. The Pt/CoFe/NF-based overall hydrazine splitting (OHzS) device can realize 10 and 100 mA cm–2 at low potential of 0.093 and 0.531 mV, respectively, and the Faradaic efficiency for both N2 and H2 generation reaches nearly 100%. Such HER and HzOR activities can be attributed to the electronic metal–support interaction (EMSI) between Pt and CoFe/NF, which modulates the d-band center of Pt to an optimal position, thereby balancing the adsorption of N2H4 molecules (ΔG*N2H4 = −2.27 eV) and the desorption of hydrogen (ΔGH* = −0.18 eV) by Pt/CoFe/NF. This work provides insights into the design of efficient bifunctional catalysts from the perspective of the electronic structure.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":11.3000,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c03881","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

Hydrazine-assisted water electrolysis presents an energy-saving pathway for H₂ production. However, due to the different electronic structure requirements for active metals in hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) reactions, catalysts capable of simultaneously driving HER and HzOR are less studied. Herein, we employ an electrochemical deposition method to load 4.2 nm Pt nanoparticles onto CoFe-layered double hydroxides. The resultant Pt/CoFe/NF requires only 12.1 and 28.7 mV to achieve 50 and 100 mA cm^–2 for HzOR and an ultralow overpotential of 16.5 mV with a Tafel slope of 31.4 mV dec^–1 to achieve 10 mA cm^–2 for HER. The Pt/CoFe/NF-based overall hydrazine splitting (OHzS) device can realize 10 and 100 mA cm^–2 at low potential of 0.093 and 0.531 mV, respectively, and the Faradaic efficiency for both N₂ and H₂ generation reaches nearly 100%. Such HER and HzOR activities can be attributed to the electronic metal–support interaction (EMSI) between Pt and CoFe/NF, which modulates the d-band center of Pt to an optimal position, thereby balancing the adsorption of N₂H₄ molecules (ΔG_*N₂H₄ = −2.27 eV) and the desorption of hydrogen (ΔG_H* = −0.18 eV) by Pt/CoFe/NF. This work provides insights into the design of efficient bifunctional catalysts from the perspective of the electronic structure.

Abstract Image

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

同时驱动 HER 和 HzOR 的铂负载 CoFe 层双氢氧化物

肼辅助水电解是一种生产 H2 的节能途径。然而，由于氢进化反应（HER）和肼氧化反应（HzOR）反应对活性金属的电子结构要求不同，能够同时驱动 HER 和 HzOR 的催化剂研究较少。在此，我们采用电化学沉积法将 4.2 纳米铂粒子负载到 CoFe 层状双氢氧化物上。由此产生的 Pt/CoFe/NF 只需要 12.1 和 28.7 mV 就能实现 50 和 100 mA cm-2 的 HzOR，而 16.5 mV 的超低过电位和 31.4 mV dec-1 的 Tafel 斜坡就能实现 10 mA cm-2 的 HER。基于 Pt/CoFe/NF 的整体肼分裂（OHzS）装置可在 0.093 和 0.531 mV 的低电位下分别实现 10 和 100 mA cm-2，N2 和 H2 生成的法拉第效率接近 100%。这种 HER 和 HzOR 活性可归因于 Pt 与 CoFe/NF 之间的电子金属支撑相互作用 (EMSI)，EMSI 可将 Pt 的 d 带中心调制到最佳位置，从而平衡 Pt/CoFe/NF 对 N2H4 分子的吸附（ΔG*N2H4 = -2.27 eV）和对氢气的解吸（ΔGH* = -0.18 eV）。这项工作从电子结构的角度为设计高效的双功能催化剂提供了启示。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文去求助

来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.