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Peer-reviewedCC BY 4.0Angewandte Chemie (International Ed. in English)

Constructing p‐d Orbital Hybridization via In Situ Generation of Bi19Br3S27/NiS x for Highly Selective Photothermal CO2 Reduction to C2H4

  1. 1Hubei Key Laboratory of Mineral Resources Processing and Environment, Key Laboratory of Green Utilization of Critical Non‐metallic Mineral Resources, Ministry of Education, State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology Wuhan People's Republic of China
  2. 2Department of Chemistry National University of Singapore Singapore Singapore

Abstract

Photothermal catalytic CO2 reduction to multi‐carbon products is a promising approach for carbon utilization, yet the design of active sites that effectively promote multistep C─C coupling toward selective C2H4 formation remains a significant challenge. Hence, we employ an in situ interfacial engineering strategy to construct crystalline/amorphous Bi19Br3S27/NiS x (BBSN) photothermal catalysts with strong p‐d orbital hybridization. The optimized BBSN‐8 achieves a C2H4 production rate of 41.38 µmol g−1 h−1 with a selectivity of 96.8% under full‐spectrum irradiation, which exhibits a remarkable advantage in the field of C2H4 production. Experimental results and theoretical calculations demonstrate that Ni incorporation optimizes CO2 adsorption from overly strong Bi─C single‐site binding to balanced multi‐sites adsorption, while newly formed p‐d orbital hybridization establishes electronically cooperative Bi─S─Ni active sites stabilizing both carbon‐ and oxygen‐centered species, synergistically facilitating *CO─CHO* coupling and boosting C2H4 formation. This work demonstrates that in situ interfacial orbital hybridization can regulate intermediate coupling and steer photothermal CO2 reduction toward highly selective C2H4 formation.

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BibTeX
@article{gan2026constructing,
  title = {{Constructing p‐d Orbital Hybridization via In Situ Generation of Bi19Br3S27/NiS x for Highly Selective Photothermal CO2 Reduction to C2H4}},
  author = {Guangmei Gan and Zhixiong Yang and Mengying Wang and Yang Shi and Yuan Li and Gaoke Zhang and Jie Wu},
  journal = {Angewandte Chemie (International Ed. in English)},
  year = {2026},
  month = sep,
  doi = {10.1002/anie.1626004},
  url = {https://doi.org/10.1002/anie.1626004},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Constructing p‐d Orbital Hybridization via In Situ Generation of Bi19Br3S27/NiS x for Highly Selective Photothermal CO2 Reduction to C2H4
AU  - Guangmei Gan
AU  - Zhixiong Yang
AU  - Mengying Wang
AU  - Yang Shi
AU  - Yuan Li
AU  - Gaoke Zhang
AU  - Jie Wu
PY  - 2026
DA  - 2026/09/15
JO  - Angewandte Chemie (International Ed. in English)
DO  - 10.1002/anie.1626004
UR  - https://doi.org/10.1002/anie.1626004
AB  - Photothermal catalytic CO2 reduction to multi‐carbon products is a promising approach for carbon utilization, yet the design of active sites that effectively promote multistep C─C coupling toward selective C2H4 formation remains a significant challenge. Hence, we employ an in situ interfacial engineering strategy to construct crystalline/amorphous Bi19Br3S27/NiS x (BBSN) photothermal catalysts with strong p‐d orbital hybridization. The optimized BBSN‐8 achieves a C2H4 production rate of 41.38 µmol g−1 h−1 with a selectivity of 96.8% under full‐spectrum irradiation, which exhibits a remarkable advantage in the field of C2H4 production. Experimental results and theoretical calculations demonstrate that Ni incorporation optimizes CO2 adsorption from overly strong Bi─C single‐site binding to balanced multi‐sites adsorption, while newly formed p‐d orbital hybridization establishes electronically cooperative Bi─S─Ni active sites stabilizing both carbon‐ and oxygen‐centered species, synergistically facilitating *CO─CHO* coupling and boosting C2H4 formation. This work demonstrates that in situ interfacial orbital hybridization can regulate intermediate coupling and steer photothermal CO2 reduction toward highly selective C2H4 formation.
SN  - 1433-7851
SN  - 1521-3773
ER  -