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Quasi-homogeneous photoelectrochemical organic transformations for tunable products and 100% conversion ratio.
Lin, Cheng; Lu, Yuan; Miao, Jiaming; Ma, Zhongyuan; Choi, Youngmoon; Yang, Yan; Dong, Chaoran; Shen, Jinyou; Park, Jong Hyeok; Zhang, Kan.
Afiliação
  • Lin C; School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
  • Lu Y; Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul 120-749, Republic of Korea.
  • Miao J; School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
  • Ma Z; Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul 120-749, Republic of Korea.
  • Choi Y; Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul 120-749, Republic of Korea.
  • Yang Y; School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
  • Dong C; Key Laboratory of Environmental Remediation and Ecological Health, Ministry of Industry and Information Technology, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
  • Shen J; Key Laboratory of Environmental Remediation and Ecological Health, Ministry of Industry and Information Technology, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China. Electronic address: shenjinyou@mail.njust.edu.cn.
  • Park JH; Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul 120-749, Republic of Korea. Electronic address: lutts@yonsei.ac.kr.
  • Zhang K; School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China. Electronic address: zhangkan@njust.edu.cn.
Sci Bull (Beijing) ; 2024 Aug 16.
Article em En | MEDLINE | ID: mdl-39181786
ABSTRACT
Photoelectrochemical (PEC) organic transformation at the anode coupled with cathodic H2 generation is a potentially rewarding strategy for efficient solar energy utilization. Nevertheless, achieving the full conversion of organic substrates with exceptional product selectivity remains a formidable hurdle in the context of heterogeneous catalysis at the solid/liquid interface. Here, we put forward a quasi-homogeneous catalysis concept by using the reactive oxygen species (ROS), such as ·OH, H2O2 and SO4•-, as a charge transfer mediator instead of direct heterogeneous catalysis at the solid/liquid interface. In the context of glycerol oxidation, all ROS exhibited a preference for first-order reaction kinetics. These ROS, however, showcased distinct oxidation mechanisms, offering a range of advantages such as âˆ¼ 100 % conversion ratios and the flexibility to tune the resulting products. Glycerol oxidative formic acid with Faradaic efficiency (FE) of 81.2 % was realized by the H2O2 and ·OH, while SO4•- was preferably for glycerol conversion to C3 products like glyceraldehyde and dihydroxyacetone with a total FE of about 80 %. Strikingly, the oxidative coupling of methane to ethanol was successfully achieved in our quasi-homogeneous system, yielding a remarkable production rate of 12.27 µmol h-1 and an impressive selectivity of 92.7 %. This study is anticipated to pave the way for novel approaches in steering solar-driven organic conversions by manipulating ROS to attain desired products and conversion ratios.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Sci Bull (Beijing) Ano de publicação: 2024 Tipo de documento: Article País de afiliação: China País de publicação: Holanda
Texto completo
Adicionar na Minha BVS
Imprimir
XML
PubMed Links
Buscar no Google

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Sci Bull (Beijing) Ano de publicação: 2024 Tipo de documento: Article País de afiliação: China País de publicação: Holanda