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Abstract
The objective of photocatalytic CO2 reduction (PCR) is to achieve high selectivity
for a single energy-bearing product with high efficiency and stability. The bulk configuration
usually determines charge carrier kinetics, whereas surface atomic arrangement defines
the PCR thermodynamic pathway. Concurrent engineering of bulk and surface structures
is therefore crucial for achieving the goal of PCR. Herein, an ultrastable and highly
selective PCR using homogeneously doped BiOCl nanosheets synthesized via an inventive
molten strategy is presented. With B2 O3 as both the molten salt and doping precursor,
this new doping approach ensures boron (B) doping from the surface into the bulk with
dual functionalities. Bulk B doping mitigates strong excitonic effects confined in
2D BiOCl by significantly reducing exciton binding energies, whereas surface-doped
B atoms reconstruct the BiOCl surface by extracting lattice hydroxyl groups, resulting
in intimate B-oxygen vacancy (B-OV) associates. These exclusive B-OV associates enable
spontaneous CO2 activation, suppress competitive hydrogen evolution and promote the
proton-coupled electron transfer step by stabilizing *COOH for selective CO generation.
As a result, the homogeneous B-doped BiOCl nanosheets exhibit 98% selectivity for
CO2 -to-CO reduction under visible light, with an impressive rate of 83.64 µmol g-1
h-1 and ultrastability for long-term testing of 120 h.
[1
]Key Laboratory of Pesticide and Chemical Biology of Ministry of Education Institute
of Environmental and Applied Chemistry College of Chemistry Central China Normal University
Wuhan 430079 P. R. China