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The Hole‐Tunneling Heterojunction of Hematite‐Based Photoanodes Accelerates Photosynthetic Reaction
Author(s) -
Zhang Hongwen,
Zhang Pu,
Zhao Jiwu,
Liu Yuan,
Huang Yi,
Huang Haowei,
Yang Chen,
Zhao Yibo,
Wu Kaifeng,
Fu Xianliang,
Jin Shengye,
Hou Yidong,
Ding Zhengxin,
Yuan Rusheng,
Roeffaers Maarten B. J.,
Zhong Shuncong,
Long Jinlin
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202102983
Subject(s) - overlayer , materials science , heterojunction , nanorod , nanotechnology , chemistry , optoelectronics
Single‐atom metal‐insulator‐semiconductor (SMIS) heterojunctions based on Sn‐doped Fe 2 O 3 nanorods (SF NRs) were designed by combining atomic deposition of an Al 2 O 3 overlayer with chemical grafting of a RuO x hole‐collector for efficient CO 2 ‐to‐syngas conversion. The RuO x ‐Al 2 O 3 ‐SF photoanode with a 3.0 nm thick Al 2 O 3 overlayer gave a >5‐fold‐enhanced IPCE value of 52.0 % under 370 nm light irradiation at 1.2 V vs. Ag/AgCl, compared to the bare SF NRs. The dielectric field mediated the charge dynamics at the Al 2 O 3 /SF NRs interface. Accumulation of long‐lived holes on the surface of the SF NRs photoabsorber aids fast tunneling transfer of hot holes to single‐atom RuO x species, accelerating the O 2 ‐evolving reaction kinetics. The maximal CO‐evolution rate of 265.3 mmol g −1 h −1 was achieved by integration of double SIMS‐3 photoanodes with a single‐atom Ni‐doped graphene CO 2 ‐reduction‐catalyst cathode; an overall quantum efficiency of 5.7 % was recorded under 450 nm light irradiation.