Multivalent Sn species synergistically favours the CO_(2)-into-HCOOH conversion  

作　　者：Jun Wu Xue Bai Zhiyu Ren Shichao Du Ziehen Song Lei Zhao Bowen Liu Guiling Wang Honggang Fu 

机构地区：[1]Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education,College of Materials Science and Chemical Engineering,Harbin Engineering University,Harbin 150001,China [2]Key Laboratory of Functional Inorganic Material Chemistry,Ministry of Education of the Peoples Republic of China,Heilongjiang University,Harbin 150080,China

出　　处：《Nano Research》2021年第4期1053-1060,共8页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(Nos.21631004,21901065);the Natural Science Foundation of Heilongjiang Province of China(No.LH2020B019);the Youth Science and Technology Innovation Team Project of Heilongjiang Province(No.RCYJTD201803);the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2018009).

摘　　要：Although Sn-based catalysts have recently achieved considerable improvement in selective electro-catalyzing CO_(2)into HCOOH,the role of various valence Sn species is not fully understood due to the complexity and uncertainty of their evolution during the reaction process.Here,inspired by the theoretical simulations that the concomitant multivalent Sn(Sn^(0),Sn^(Ⅱ)and Sn^(Ⅳ))can significantly motivate the intrinsic activity of Sn-based catalyst,the Sn/SnO/SnO_(2)nanosheets were proposed to experimentally verify the synergistic effect of multivalent Sn species on the CO_(2)-into-HCOOH conversion.During CO_(2)reduction reaction,the Sn/SnO/SnO_(2)nanosheets,which are prepared by the sequential hydrothermal reaction,calcined crystallization and low-temperature H_(2)treatment,exhibit a high FEHCOOH of 89.6%at-0.9 VRHE as well as a large cathodic current density.Systematic experimental and theoretical results corroborate that multivalent Sn species synergistically energize the CO_(2)activation,the HCOO*adsorption,and the electron transfer,which make Sn/SnO/SnO_(2)favour the conversion from CO_(2)into HCOOH in both thermodynamics and kinetics.This proof-of-concept study establishes a relationship between the enhanced performance and the multivalent Sn species,and also provides a practicable and scalable avenue for rational engineering high-powered electrocatalysts.

关 键 词：CO_(2)reduction ELECTROCATALYTIC formic acid multivalent Sn density functional theory(DFT)calculation 

分 类 号：O64[理学—物理化学]