Boosted Charge Transfer for Highly Efficient Photosynthesis of H2O2 over Z‐Scheme I−/K+ Co‐Doped g‐C3N4/Metal–Organic‐Frameworks in Pure Water under Visible Light
Source abstract
Abstract
Abstract Photocatalytic oxygen reduction reaction (ORR) is an environmentally friendly and cost‐effective approach for H2O2 synthesis. However, the current photosynthesis system suffers from sluggish kinetics, rapid recombination of photoexcited charge carriers, and weak redox potentials, resulting in unsatisfactory solar‐to‐chemical conversion efficiency. Herein, a Z‐scheme heterojunction (UiO/IKCN) is constructed through coupling I−/K+ co‐doped g‐C3N4 (IKCN) with NH2‐UiO‐66, a typical metal‐organic framework material. Under visible light irradiation, the optimal UiO/IKCN exhibits exceptional H2O2 production rates in pure water (13.3 mM g−1 h−1) and in isopropanol solution (72.6 mM g−1 h−1), that is 48.4 times higher than pristine CN in isopropanol (1.5 mM g−1 h−1). A high apparent quantum yield of 10.28% at 420 nm is achieved by UiO/IKCN, surpassing most previously reported values. The dominating role of two‐electron ORR in H2O2 photosynthesis is elucidated in detail. The significantly enhanced photocatalytic activity can be attributed to the facilitated charge separation and Z‐scheme charge transfer, which are unambiguously verified by stable‐state surface photovoltage, transient photoluminescence, femtosecond transient absorption spectroscopy, in‐situ irradiated X‐ray photoelectron spectroscopy, and density functional theory calculations. This study represents the first exploration of H2O2 production using NH2‐UiO‐66 and provides insights into the rational design of Z‐scheme heterojunction for highly efficient photosynthesis.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Advanced Photocatalysis Techniques · Perovskite Materials and Applications · Copper-based nanomaterials and applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Shandong Key Laboratory of Environmental Processes and Health School of Environmental Science and Engineering Shandong University Qingdao 266237 China
Henan Institute of Advanced Technology Zhengzhou University Zhengzhou 450052 China
School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat‐sen University Guangzhou 510006 China
Research Center for Particle Science and Technology Institute of Frontier and Interdisciplinary Science Shandong University Qingdao 266237 China
State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco‐Environmental Sciences Chinese Academy of Sciences Beijing 10085 China
Department of Chemistry and Biochemistry Florida International University Miami Florida 33199 USA
Centre Énergie Materiaux et Télécommunications Institut National de la Recherche Scientifique (INRS) Varennes Québec J3X 1P7 Canada
Funding
National Natural Science Foundation of China · Natural Sciences and Engineering Research Council of Canada · Canada Research Chairs · Basic and Applied Basic Research Foundation of Guangdong Province · Taishan Scholar Foundation of Shandong Province · Natural Science Foundation of Shandong Province
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