Journal article
Asymmetric atomic-level engineering of phosphorus-modified Cu single-atom coordination centers on carbon nitride for enhanced photocatalytic hydrogen evolution
Chemical science (Cambridge)
30 Jul 2026
PMID: 42568865
Abstract
Single-atom photocatalysts (SACs) have emerged as an effective strategy for enhancing solar energy conversion by improving light absorption and charge carrier dynamics; however, precise construction of isolated active sites remains challenging. Herein, we report atomically dispersed Cu single atoms uniformly anchored on phosphorus-doped graphitic carbon nitride (Cu-PCN). The optimized catalyst achieves an excellent hydrogen evolution rate of 3276 µmol g−1 h−1 with an apparent quantum yield (AQY) of 31% at 400 nm, surpassing most reported metal–N coordinated systems. X-ray absorption spectroscopy (XAS) confirms the atomic dispersion and defined coordination of Cu single atoms within the g-C3N4 framework. Combined experimental and theoretical studies reveal that the Cu sites extend light absorption, enhance charge separation and interfacial transfer, and promote H2O activation by guiding electron migration toward Cu centers with reduced energy barriers, thereby facilitating the formation of H* intermediates as the crucial step in hydrogen evolution. Overall, this work demonstrates an effective approach to engineer asymmetric active sites via coordination tuning, providing valuable insights for designing efficient photocatalysts for solar-driven hydrogen evolution reaction. Asymmetric atomic-level engineering and synergistic interactions between adjacent sites significantly enhance photocatalytic hydrogen evolution by improving light absorption and charge-carrier dynamics.
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- Title
- Asymmetric atomic-level engineering of phosphorus-modified Cu single-atom coordination centers on carbon nitride for enhanced photocatalytic hydrogen evolution
- Creators
- Hafijul Islam - Indian Institute of Chemical TechnologyBhavya Jaksani - Indian Institute of Chemical TechnologySaad Mehmood - Indian Institute of Chemical TechnologySukanya Saha - Indian Institute of Chemical TechnologyBidyut Bikash Sarma - Centre National de la Recherche ScientifiqueB. Moses Abraham - A. J. Drexel Nanomaterials Institute, Department of Materials Science and Engineering, Drexel University Department of Chemical Engineering, Indian Institute of Technology KanpurUjjwal Pal - Indian Institute of Chemical Technology
- Publication Details
- Chemical science (Cambridge)
- Publisher
- Royal Society of Chemistry
- Number of pages
- 11
- Grant note
- Academy of Scientific and Innovative Research: Unassigned University Grants Commission: Unassigned National Institute of Ocean Technology, Ministry of Earth Sciences: GAP-1086 Council of Scientific and Industrial Research, India: IICT/Pubs./2026/155 Hindustan Petroleum: CLP-0138
This work was supported by MoES-NIOT, New Delhi (Project no: GAP-1086) and HPCL (Project no: CLP-0138/HPCL). H. I. thanks AcSIR for PhD enrollment and UGC for financial support (CSIR-IICT Communication No. IICT/Pubs./2026/155). B. B. S would like to acknowledge DESY synchrotron (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of beamtime. This research was carried out at the P65 beamline of PETRA III (proposal number I-20250952 EC).
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering
- Web of Science ID
- WOS:001842519100001
- Other Identifier
- 991022201580204721