Affiliation:
1. Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of Education Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China
2. College of Chemistry and Chemical Engineering Central South University Changsha Hunan 410083 China
3. Department of Chemistry and Biochemistry The Ohio State University Columbus Ohio 43210 USA
Abstract
AbstractAcidic water electrolysis (AWE) has the potential to revolutionize green H2 generation with flexible partial load range, high gas purity, and rapid system response. However, the extensive usage of noble Ru/Ir metals and sluggish oxygen evolution reaction (OER) with inexpensive O2 products pose significant challenges in anodes. Herein, it is demonstrated that ultralow Pt single atoms in highly porous N‐doped carbons (Pt1/p‐NC@CNTs) can effectively catalyze chlorine evolution reaction (CER) for on‐site chlorination to replace OER in AWE, with 200 mV potential saving at 10 mA cm−2. As a result, various organic halide motifs of pharmaceutical molecules by chlorinating anisole, ketones, and olefins can be realized, along with H2 coproduction. Combined physicochemical characterizations including synchrotron X‐ray absorption spectroscopy, finite element methodsimulations, and theory calculations indicate that atomic Pt‐N4 active sites balance the adsorption/desorption of Cl intermediates (Volmer step) and the plentiful porosity of Pt1/p‐NC@CNTs with high specific surface area of 313 m2 g−1 enriches Cl− around active sites (Heyrovský step), collectively promoting the rate‐limiting Volmer–Heyrovský pathway for improved CER.
Funder
National Key Research and Development Program of China
National Natural Science Foundation of China
Natural Science Foundation of Hunan Province
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials
Cited by
7 articles.
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