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Visible Light-Driven Conversion of Carbon-Sequestrated Seawater into Stoichiometric CO and HClO with Nitrogen-Doped BiOCl Atomic Layers
Authors:Yanbiao Shi  Hongwei Shou  Hao Li  Guangming Zhan  Xupeng Liu  Zhiping Yang  Chengliang Mao  Jundi Cheng  Xu Zhang  Yaqian Jiang  Shengxi Zhao  Jiaxian Wang  Prof Xiao Liu  Prof Li Song  Hongwei Sun  Prof Lizhi Zhang
Institution:1. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P. R. China;2. National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230029 P. R. China

These authors contributed equally to this work.

Contribution: Software (lead);3. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P. R. China

Contribution: Software (supporting);4. Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China

Contribution: ​Investigation (supporting);5. Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Departments of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON, M5S 3H6 Canada

Contribution: ​Investigation (supporting);6. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P. R. China

Contribution: ​Investigation (supporting);7. National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230029 P. R. China

Contribution: Software (supporting);8. Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China

Abstract:Seawater is one of the most important CO2 sequestration media for delivering value-added chemicals/fuels and active chlorine; however, this scenario is plagued by sluggish reaction rates and poor product selectivity. Herein, we first report the synthesis of nitrogen-doped BiOCl atomic layers to directly split carbon-sequestrated natural seawater (Yellow Sea, China) into stoichiometric CO (92.8 μmol h−1) and HClO (83.2 μmol h−1) under visible light with selectivities greater than 90 %. Photoelectrons enriched on the exposed BiOCl{001} facet kinetically facilitate CO2-to-CO reduction via surface-doped nitrogen bearing Lewis basicity. Photoholes, mainly located on the lateral facets of van der Waals gaps, promote the selective oxidation of Cl into HClO. Sequestrated CO2 also maintains the pH of seawater at around 4.2 to prevent the alkaline earth cations from precipitating. The produced HClO can effectively kill typical bacteria in the ballast water of ocean-going cargo ships, offering a green and safe way for onsite sterilization.
Keywords:Active Chlorine  CO2 Reduction  Carbon Sequestration  Photocatalysis  Seawater
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