Affiliation:
1. State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials PSU-DUT Joint Center for Energy Research School of Chemical Engineering Dalian University of Technology Dalian 116024 China
2. Department of Chemistry Faculty of Science The Chinese University of Hong Kong Shatin, NT Hong Kong China
Abstract
AbstractIn this work, density functional theory (DFT) calculations were conducted to investigate a series of transition metals (Cr, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Ru, Rh, Pd, Ag, Hf, Ta, Os, Ir, and Pt) as single‐atom components introduced into Ti‐BPDC (BPDC=2,2′‐bipyridine‐5,5′‐dicarboxylic acid) as catalysts (M/Ti‐BPDC) for the photocatalytic reduction of CO2. The results show that Fe/Ti‐BPDC is the most active candidate for CO2 reduction to HCOOH due to its small limiting potential (−0.40 V). Ag, Cr, Mn, Ru, Zr, Nb, Rh, and Cu modified Ti‐BPDC are also active to HCOOH since their limiting potentials are moderate although the reaction mechanisms are different across these materials. Most of the studied catalysts show poor activity and selectivity to CO product because the stability of *COOH/*OCOH intermediates is significantly weaker than *OCHO/*HCOO species. The moderate binding strength of *CO on Pd/Ti‐BPDC is responsible for its superior catalytic activity toward CH3OH generation. Electronic structural analysis was performed to uncover the origin of the activity trend for CO2 reduction to different products on M/Ti‐BPDC. The calculation results indicate that the activity and selectivity of CO2 photoreduction can be effectively tuned by designing single‐atom metal‐based MOF catalysts.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Liaoning Province
Liaoning Revitalization Talents Program
Fundamental Research Funds for the Central Universities
Subject
General Energy,General Materials Science,General Chemical Engineering,Environmental Chemistry
Cited by
2 articles.
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