Modified electronic structure and enhanced hydroxyl adsorption make quaternary Pt-based nanosheets efficient anode electrocatalysts for formic acid-/alcohol-air fuel cells  

作　　者：Fengling Zhao Qiang Yuan Siyang Nie Liang Wu Xun Wang 

机构地区：[1]State-Local Joint Laboratory for Comprehensive Utilization of Biomass,Center for R&D of Fine Chemicals,College of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,Guizhou,China [2]Key Lab of Organic Optoelectronics&Molecular Engineering,Tsinghua University,Beijing 100084,China [3]School of Chemistry and Chemical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China

出　　处：《Journal of Energy Chemistry》2024年第5期142-150,共9页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(21571038,22035004);the Education Department of Guizhou Province(2021312);the Foundation of Guizhou Province(2019-5666);the National Key R&D Program of China(2017YFA0700101);the State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University,202009)。

摘　　要：Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.

关 键 词：Pt-based nanosheets Modifiedelectronic structure Enhanced hydroxyl adsorption Formicacidand alcohol oxidation Direct liquid fuel cells 

分 类 号：TB383.1[一般工业技术—材料科学与工程] TQ426[化学工程] TM911.4[电气工程—电力电子与电力传动]