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Cheng Tang, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth R. Davey, Shi‐Zhang Qiao
Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback is the limited understanding of actual catalytic active sites. Here, using as a prototype single-atom catalysts (SACs) in acidic oxygen reduction reaction (ORR), we report the structure–property relationship of catalysts and show for the first time that molecular-level local structure, including first and second coordination spheres (CSs), rather than individual active atoms, synergistically determines the electrocatalytic response. ORR selectivity on Co-SACs can be tailored from a four-electron to a two-electron pathway by modifying first (N or/and O coordination) and second (C–O–C groups) CSs. Using combined theoretical predictions and experiments, including X-ray absorption fine structure analyses and in situ infrared spectroscopy, we confirm that the unique selectivity change originates from the structure-dependent shift of active sites from the center Co atom to the O-adjacent C atom. We show this optimizes the electronic structure and *OOH adsorption behavior on active sites to give the present “best” activity and selectivity of >95% for acidic H 2 O 2 electrosynthesis.
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Tang, C., Chen, L., Li, H., Li, L., Jiao, Y., Zheng, Y., Xu, H., Davey, K. R., & Qiao, S. (2021). Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres. Journal of the American Chemical Society, 143(20), 7819–7827. https://doi.org/10.1021/jacs.1c03135
Tang, Cheng, et al. "Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres." Journal of the American Chemical Society, vol. 143, no. 20, 2021, pp. 7819–7827, https://doi.org/10.1021/jacs.1c03135.
Tang, Cheng, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth R. Davey, and Shi‐Zhang Qiao. "Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres." Journal of the American Chemical Society 143, no. 20 (2021): 7819–7827. https://doi.org/10.1021/jacs.1c03135.
Tang C., Chen L., Li H. [и др.] Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres // Journal of the American Chemical Society. — 2021. — Vol. 143, № 20. — P. 7819–7827. — URL: https://doi.org/10.1021/jacs.1c03135
@article{tang2021tailoring,
title = {{Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres}},
author = {Cheng Tang and Ling Chen and Haijing Li and Laiquan Li and Yan Jiao and Yao Zheng and Haolan Xu and Kenneth R. Davey and Shi‐Zhang Qiao},
journal = {Journal of the American Chemical Society},
year = {2021},
volume = {143},
number = {20},
pages = {7819--7827},
doi = {10.1021/jacs.1c03135},
url = {https://doi.org/10.1021/jacs.1c03135}
}TY - JOUR AU - Tang, Cheng AU - Chen, Ling AU - Li, Haijing AU - Li, Laiquan AU - Jiao, Yan AU - Zheng, Yao AU - Xu, Haolan AU - Davey, Kenneth R. AU - Qiao, Shi‐Zhang TI - Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres JO - Journal of the American Chemical Society VL - 143 IS - 20 SP - 7819 EP - 7827 PY - 2021 DA - 2021/05/13 DO - 10.1021/jacs.1c03135 UR - https://doi.org/10.1021/jacs.1c03135 ER -
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