Room-temperature Photosynthesis of Propane from CO with Cu Single Atoms on Vacancy-rich TiO

Overview

Journal Nat Commun

Specialty Biology

Date 2023 Feb 27

PMID 36849519

Authors

Yan Shen

Chunjin Ren

Lirong Zheng

Xiaoyong Xu

Ran Long

Wenqing Zhang

Yong Yang

Yongcai Zhang

Yingfang Yao

Haoqiang Chi

Jinlan Wang

Qing Shen

Yujie Xiong

Zhigang Zou

Yong Zhou

Affiliations

Soon will be listed here.

Abstract

Photochemical conversion of CO into high-value C products is difficult to achieve due to the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for the conversion of CO into CH is prepared by implanting Cu single atoms on TiO atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (Vs) in TiO matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-V unit in TiO matrix. A high electron-based selectivity of 64.8% for CH (product-based selectivity of 32.4%), and 86.2% for total C hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-V unit may stabilize the key *CHOCO and *CHOCOCO intermediates and reduce their energy levels, tuning both C-C and C-C couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are tentatively proposed for CH formation, involving an overall (20e - 20H) reduction and coupling of three CO molecules at room temperature.

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