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|Title:||Tailoring acidic oxygen reduction selectivity on single-atom catalysts via modification of first and second coordination spheres|
|Citation:||Journal of the American Chemical Society, 2021; 43(20):4819-4827|
|Publisher:||American Chemical Society (ACS)|
|Cheng Tang, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth Davey, and Shi-Zhang Qiao|
|Abstract:||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 H₂O₂ electrosynthesis.|
|Rights:||© 2021 American Chemical Society|
|Appears in Collections:||Aurora harvest 8|
Chemical Engineering publications
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