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Highly Selective Photoreduction of CO 2 with Suppressing H 2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm
Author(s) -
Tan Ling,
Xu SiMin,
Wang Zelin,
Xu Yanqi,
Wang Xian,
Hao Xiaojie,
Bai Sha,
Ning Chenjun,
Wang Yu,
Zhang Wenkai,
Jo Yun Kyung,
Hwang SeongJu,
Cao Xingzhong,
Zheng Xusheng,
Yan Hong,
Zhao Yufei,
Duan Haohong,
Song YuFei
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201904246
Subject(s) - hydroxide , monolayer , irradiation , photochemistry , photocatalysis , ruthenium , selectivity , materials science , photosensitizer , chemistry , catalysis , visible spectrum , nanotechnology , inorganic chemistry , optoelectronics , physics , nuclear physics , biochemistry
Although progress has been made to improve photocatalytic CO 2 reduction under visible light ( λ >400 nm), the development of photocatalysts that can work under a longer wavelength ( λ >600 nm) remains a challenge. Now, a heterogeneous photocatalyst system consisting of a ruthenium complex and a monolayer nickel‐alumina layered double hydroxide (NiAl‐LDH), which act as light‐harvesting and catalytic units for selective photoreduction of CO 2 and H 2 O into CH 4 and CO under irradiation with λ >400 nm. By precisely tuning the irradiation wavelength, the selectivity of CH 4 can be improved to 70.3 %, and the H 2 evolution reaction can be completely suppressed under irradiation with λ >600 nm. The photogenerated electrons matching the energy levels of photosensitizer and m‐NiAl‐LDH only localized at the defect state, providing a driving force of 0.313 eV to overcome the Gibbs free energy barrier of CO 2 reduction to CH 4 (0.127 eV), rather than that for H 2 evolution (0.425 eV).