P-tuned FeN_(2)binuclear sites for boosted CO_(2)electro-reduction  

作　　者：Cao Guo Sanshuang Gao Jun Li Menglin Zhou Abdukader Abdukayum Qingquan Kong Yingtang Zhou Guangzhi Hu 

机构地区：[1]School of Materials and Energy,Institute for Ecological Research and Pollution Control of Plateau Lakes,School of Ecology and Environmental Science,Yunnan University,Kunming 650504,Yunnan,China [2]Xinjiang Key Laboratory of Novel Functional Materials Chemistry,College of Chemistry and Environmental Sciences,Kashi University,Kashi 844000,Xinjiang,China [3]School of Mechanical Engineering,Chengdu University,Chengdu 610106,Sichuan,China [4]National Engineering Research Center for Marine Aquaculture,Marine Science and Technology College,Zhejiang Ocean University,Zhoushan 316004,Zhejiang,China

出　　处：《Journal of Energy Chemistry》2025年第2期816-824,I0018,共10页能源化学(英文版)

基　　金：financially supported by the National Natural Science Foundation of China-Yunnan Joint Fund(U2002213);Science and Technology Talent and Platform Program of Yunnan Provincial Science and Technology Department(202305AM070001);the Xingdian Talent Program of Yunnan Province;the Double-First Class University Plan(C176220100042).

摘　　要：The recycling of CO_(2)through electrochemical processes offers a promising solution for alleviating the greenhouse effect;however,the activation of CO_(2)and desorption of^(*)CO in electrocatalytic CO_(2)reduction(ECR)frequently encounter high energy barriers and competitive hydrogen evolution reactions(HERs),which are urgent problems that need to be addressed.In this study,a catalyst(P100-Fe-N/C)with homogeneous P-tuned FeN_(2)binuclear sites(N_(2)PFe-FePN_(2))was successfully synthesised,demonstrating satisfactory performance in the ECR to CO.P100-Fe-N/C attains a peak FECOof 98.01%and a normalized TOF of 664.7 h-1at-0.7 VRHE,surpassing the performance of the Fe binuclear catalyst without P and singleatoms catalysts.In the MEA cell,a FECOexceeding 90%can still be achieved.Density functional theory analysis indicates that the asymmetric coordination configuration induced by the incorporation of P facilitates a reduction in the system's energy.The modulation of P results in the d-band centre of the catalyst being positioned closer to the Fermi level,which facilitates the interaction of the catalyst with CO_(2),allowing more electrons to be injected into the CO_(2)molecule at the Fe binuclear sites and inhibiting the HER.The P-tuned FeN_(2)binuclear sites effectively lower the^(*)CO desorption barrier.

关 键 词：Electrocatalysis Diatomic catalyst Heteroatom doping CO_(2)reduction reaction DFT calculation 

分 类 号：O62[理学—有机化学]