文献类型：期刊文献

英文题名：Stable Ni(II) sites in Prussian blue analogue for selective, ampere-level ethylene glycol electrooxidation

作者：Liu, Ji Kai[1];Kang, Mengde[2];Huang, Kai[2];Xu, Hao Guan[1];Wu, Yi Xiao[1];Zhang, Xin Yu[3,4];Zhu, Yan[1];Fan, Hao[1];Fang, Song Ru[1];Zhou, Yi[3];Lian, Cheng[2];Liu, Peng Fei[1,4];Yang, Hua Gui[1,4]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Minist Educ,Key Lab Ultrafine Mat, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai, Peoples R China;[3]East China Univ Sci & Technol, Sch Resources & Environm Engn, Dept Energy & Chem Engn, Shanghai, Peoples R China;[4]Minist Educ, Engn Res Ctr Resource Utilizat Carbon containing W, Shanghai, Peoples R China

年份：2025

卷号：16

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001463754400001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (22239001, 22379043, 51920105003 and 22309053), the Shanghai Pilot Program for Basic Research (22TQ1400100-12), the Science and Technology Commission of Shanghai Municipality (23520710700, 21DZ1207101 and 22ZR1415700), and the Fundamental Research Funds for the Central Universities. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) for their constructive assistance with the XAFS measurements and data analyses.

语种：英文

摘要：The industrial implementation of coupled electrochemical hydrogen production systems necessitates high power density and high product selectivity for economic viability and safety. However, for organic nucleophiles (e.g., methanol, urea, and amine) electrooxidation in the anode, most catalytic materials undergo unavoidable reconstruction to generate high-valent metal sites under harsh operation conditions, resulting in competition with oxygen evolution reaction. Here, we present unique Ni(II) sites in Prussian blue analogue (NiFe-sc-PBA) that serve as stable, efficient and selective active sites for ethylene glycol (EG) electrooxidation to formic acid, particularly at ampere-level current densities. Our in situ/operando characterizations demonstrate the robustness of Ni(II) sites during EG electrooxidation. Molecular dynamics simulations further illustrate that EG molecule tends to accumulate on the NiFe-sc-PBA surface, preventing hydroxyl-induced reconstruction in alkaline solutions. The stable Ni(II) sites in NiFe-sc-PBA anodes exhibit efficient and selective EG electrooxidation performance in a coupled electrochemical hydrogen production flow cell, producing high-value formic acid compared to traditional alkaline water splitting. The coupled system can continuously operate at stepwise ampere-level current densities (switchable 1.0 or 1.5 A cm-2) for over 500 hours without performance degradation.