Xiaohong Tan, Jiarui Wang, Yuhang Xiao, Yingying Guo, Weidong He, Binjie Du, Hao Cui, Chengxin Wang
{"title":"Engineering Topological and Chemical Disorder in Pd Sites for Record-Breaking Formic Acid Electrocatalytic Oxidation","authors":"Xiaohong Tan, Jiarui Wang, Yuhang Xiao, Yingying Guo, Weidong He, Binjie Du, Hao Cui, Chengxin Wang","doi":"10.1002/adma.202414283","DOIUrl":null,"url":null,"abstract":"Designing palladium-based formic acid oxidation reaction (FAOR) catalysts to achieve significant breakthroughs in catalytic activity, pathway selectivity, and toxicity resistance is both urgent and challenging. Here, these challenges are addressed by pioneering a novel catalyst design that incorporates both topological and chemical disorder, developing a new class of PdCuLaYMnW high-entropy amorphous alloys with a porous network (Net-Pd-HEAA) as a highly active, selective, and stable FAOR electrocatalyst. This novel Net-Pd-HEAA demonstrates record-breaking FAOR performance, achieving the mass and specific activities of 5.94 A mg<sub>Pd</sub><sup>−1</sup> and 8.94 mA cm<sup>−2</sup>, respectively, surpassing all previously reported Pd-based catalysts and showing strong competitiveness against advanced Pt-based catalysts. Simulataneously, Net-Pd-HEAA exhibits extraordinary stability in accelerated durability tests (ADT) and chronoamperometry (CA) tests. Advanced characterization and in situ, spectral analysis reveal that the extremely disordered atomic structure effectively regulates the geometric and electronic structure of the Pd sites, enhancing active intermediate coverage, facilitating dehydrogenation pathway, and inhibiting the production/adsorption of CO. Furthermore, when employed as the anode catalyst in proton exchange membrane water electrolysis (PEMWE), Net-Pd-HEAA only requires a potential of 1.28 V to obtain a current density of 1 A cm<sup>−2</sup>, and operates stably in a highly corrosive electrolyte for over 100 h.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202414283","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Designing palladium-based formic acid oxidation reaction (FAOR) catalysts to achieve significant breakthroughs in catalytic activity, pathway selectivity, and toxicity resistance is both urgent and challenging. Here, these challenges are addressed by pioneering a novel catalyst design that incorporates both topological and chemical disorder, developing a new class of PdCuLaYMnW high-entropy amorphous alloys with a porous network (Net-Pd-HEAA) as a highly active, selective, and stable FAOR electrocatalyst. This novel Net-Pd-HEAA demonstrates record-breaking FAOR performance, achieving the mass and specific activities of 5.94 A mgPd−1 and 8.94 mA cm−2, respectively, surpassing all previously reported Pd-based catalysts and showing strong competitiveness against advanced Pt-based catalysts. Simulataneously, Net-Pd-HEAA exhibits extraordinary stability in accelerated durability tests (ADT) and chronoamperometry (CA) tests. Advanced characterization and in situ, spectral analysis reveal that the extremely disordered atomic structure effectively regulates the geometric and electronic structure of the Pd sites, enhancing active intermediate coverage, facilitating dehydrogenation pathway, and inhibiting the production/adsorption of CO. Furthermore, when employed as the anode catalyst in proton exchange membrane water electrolysis (PEMWE), Net-Pd-HEAA only requires a potential of 1.28 V to obtain a current density of 1 A cm−2, and operates stably in a highly corrosive electrolyte for over 100 h.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.