文献类型：期刊文献

英文题名：Achieving high-efficient urea oxidation via regulating the rate-determining step over a V single atom incorporated Co hydroxide electrocatalyst

作者：Zhang, Baojie[1];Pan, Changti[1];Liu, Hengjie[2];Wu, Xingshun[1];Jiang, Hongliang[3];Yang, Li[1];Qi, Zeming[2];Li, Guang[1];Shan, Lei[1];Lin, Yunxiang[1];Song, Li[2];Jiang, Yong[4,5]

机构：[1]Anhui Univ, Inst Phys Sci & Informat Technol, Sch Mat Sci & Engn, Anhui Key Lab Informat Mat & Device, Hefei 230601, Peoples R China;[2]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[4]Univ Sci & Technol Beijing, Sch Mat Sci & Engn, Beijing 100083, Peoples R China;[5]Tiangong Univ, Sch Elect & Informat Engn, Tianjin 300387, Peoples R China

年份：2022

卷号：439

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20221211805759);WOS:【SCI-EXPANDED(收录号:WOS:000783147100004)】；

基金：This work is financially supported by National Key R&D Program of China (2017YFA0403503), National Natural Science Foundation of China (11674001, 21803063), Open fund for Discipline Construction, Institute of Physical Science and Information Technology (S01003103, Anhui University), the Recruitment Program for Leading Talent Team of Anhui Province (LTIT20200002), the Fundamental Research Funds for the Central Universities (WK2310000099), the Users with Excellence Program of Hefei Science Center CAS (2020HSC-UE003). We thank the National Synchrotron Radiation Laboratory (Infrared spectroscopy and microspectroscopy, MCD endstation, NSRL), Shanghai synchrotron radiation facility (SSRF, BL14W1) and Beijing synchrotron radiation facility (BSRF, 1W1B) for their experimental help.

语种：英文

外文关键词：Urea oxidation reaction; Single atom catalyst; Operando characterization; Catalytic mechanism; Rate-determining step regulation

摘要：Urea oxidation reaction (UOR) has emerged as a competitive approach for many energy-related technologies due to the low overpotential and fast reaction dynamics. The main challenge lies in fabricating high-efficient catalysts with optimized electronic structure and understanding the intrinsic structure-related mechanisms. Here, we report a feasible strategy of regulating the rate-determining step (RDS) of UOR via an electrochemical reconstructed Co hydroxide catalyst incorporated with V single atoms. The optimal catalysts exhibit an enhanced UOR performance after V incorporation while remarkably suppressed the competitive oxygen evolution with the potential of 1.54 V (vs RHE) to achieve the current density of 30 mA cm(-2). Operando synchrotron-radiation Fourier transform infrared spectroscopy (SR-FTIR) combining density functional theory (DFT) calculations reveal that enabled by single atom V incorporation, the RDS of UOR has been changed from the first deprotonation step to the second one with a lower energy barrier of 2.05 eV (vs 2.6 eV), which is thermodynamically favorable for the overall reaction process.