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“Single-atom” catalysts (SACs) have demonstrated excellent activity and selectivity in challenging chemical transformations such as photocatalytic CO 2 reduction. For heterogeneous photocatalytic SAC systems, it is essential to obtain sufficient information of their structure at the atomic level in order to understand reaction mechanisms. In this work, a SAC was prepared by grafting a molecular cobalt catalyst on a light-absorbing carbon nitride surface. Due to the sensitivity of the X-ray absorption near edge structure (XANES) spectra to subtle variances in the Co SAC structure in reaction conditions, different machine learning (ML) methods, including principal component analysis, K-means clustering, and neural network (NN), were utilized for in situ Co XANES data analysis. As a result, we obtained quantitative structural information of the SAC nearest atomic environment, thereby extending the NN-XANES approach previously demonstrated for nanoparticles and size-selective clusters.
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This content will become publicly available on April 17, 2026
Enhanced Solar CO2 Reduction Using Single Cobalt Sites on Carbon Nitride Modified with a Dianhydride
Photoactive single-atom catalysts (SACs) are among the most exciting catalytic materials for solar fuel production. Different SACs, including our own Co SACs, have been prepared on graphitic carbon nitride (C3N4) for use in photocatalysis. Building on our prior success, we report here doped C3N4 using various supplemental carbon dopants as the support for Co SACs. The Co SAC on a dianhydride doped C3N4 showed the highest activity in photocatalytic CO2 reduction. Catalyst characterization was carried out to explore the origin of the enhanced activity of this particular Co SAC. The dianhydride doped C3N4 possesses unique microstructural features, including large inter-layer space and fibrous morphology, that could contribute to the enhanced photocatalytic activity. Our results further indicate that the dianhydride is the most effective dopant to incorporate aromatic moieties in C3N4, which resulted in improved charge separation and enhanced activity in photocatalysis.
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- PAR ID:
- 10616017
- Publisher / Repository:
- American Chemical Society
- Date Published:
- Journal Name:
- The Journal of Physical Chemistry C
- Volume:
- 129
- Issue:
- 15
- ISSN:
- 1932-7447
- Page Range / eLocation ID:
- 7327 to 7334
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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