文献类型：期刊文献

英文题名：Artificial spherical chromatophore nanomicelles for selective CO2 reduction in water

作者：Yu, Junlai[1,2];Huang, Libei[3];Tang, Qingxuan[1];Yu, Shang-Bo[1];Qi, Qiao-Yan[1];Zhang, Jiangshan[2];Ma, Danying[2];Lei, Yifei[2];Su, Jianjun[3];Song, Yun[3];Eloi, Jean-Charles[4];Harniman, Robert L.[4];Borucu, Ufuk[5];Zhang, Long[6];Zhu, Minghui[7];Tian, Feng[8];Du, Lili[9,10];Phillips, David Lee[9];Manners, Ian[11];Ye, Ruquan[3,12];Tian, Jia[1]

机构：[1]Univ Chinese Acad Sci, Chinese Acad Sci, Shanghai Inst Organ Chem, Key Lab Synth & Self Assembly Chem Organ Funct Mol, Shanghai, Peoples R China;[2]Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai, Peoples R China;[3]City Univ Hong Kong, Dept Chem, State Key Lab Marine Pollut, Hong Kong, Peoples R China;[4]Univ Bristol, Sch Chem, Bristol, England;[5]Univ Bristol, Facil High Resolut Elect Cryo Microscopy GW4, Bristol, England;[6]Northwestern Univ, Dept Chem, Evanston, IL USA;[7]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai, Peoples R China;[8]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai, Peoples R China;[9]Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China;[10]Jiangsu Univ, Sch Life Sci, Zhenjiang, Peoples R China;[11]Univ Victoria, Dept Chem, Victoria, BC, Canada;[12]City Univ Hong Kong, Shenzhen Res Inst, Shenzhen, Peoples R China

年份：2023

卷号：6

期号：6

起止页码：464

外文期刊名：NATURE CATALYSIS

收录：;EI(收录号：20232114122502);WOS:【SCI-EXPANDED(收录号:WOS:000992118200001)】；

基金：J.T. acknowledges the funding support from National Key Research and Development Program of China (2022YFA1206200); Shanghai Institute of Organic Chemistry and Shanghai Branch, CAS; Shanghai Rising-Star Program (22QA1411200); and the National Natural Science Foundation of China (no. 22271306). J.T. acknowledges the Marie-Curie Fellowship. I.M. acknowledges the Canada 150 Research Chair and NSERC Discovery Grant. R.Y. acknowledges the funding support from Young Scientists Fund of the National Natural Science Foundation of China (grant no. 21905240); the Shenzhen Research Institute, City University of Hong Kong; the State Key Laboratory of Marine Pollution (SKLMP) Seed Collaborative Research Fund; the Guangdong Basic and Applied Basic Research Fund (2022A1515011333); the Shenzhen Science and Technology Program (JCYJ20220818101204009); Hong Kong Research Grant Council (21300620) and the State Key Laboratory of Marine Pollution Internal Research Fund (SKLMP/IRF/0029). D.L.P. and L.D. thank the University of Hong Kong Development Fund 2013-2014 project 'New Ultrafast Spectroscopy Experiments for Shared Facilities'. We thank the Shanghai Synchrotron Radiation Facility for providing the BL16B1 and BL10U1 beamline for collecting the synchrotron X-ray scattering data. We acknowledge access and support of the GW4 Facility for High-Resolution Electron Cryo-Microscopy, funded by the Wellcome Trust (202904/Z/16/Z and 206181/Z/17/Z) and BBSRC (BB/R000484/1). We thank Y. Zhang and X. Jin for the useful discussions. We thank M. Sener and D. H. Fackler for permission to use the visual molecular dynamics model in Fig. 1c.

语种：英文

外文关键词：Antennas - Artificial photosynthesis - Carbon dioxide - Catalyst selectivity - Solar fuels - Spheres

摘要：In nature, photosynthetic organelles harness solar radiation to produce energy-rich compounds from water and atmospheric CO2 via exquisite supramolecular assemblies. Although artificial photocatalytic cycles have been shown to occur at higher intrinsic efficiencies, the low selectivity and stability in water for multi-electron CO(2 )reduction hamper their practical applications. The creation of water-compatible artificial photocatalytic systems mimicking the natural photosynthetic apparatus for selective and efficient solar fuel production represents a major challenge. Here we show a highly stable and efficient artificial spherical chromatophore nanomicelle system self-assembled from Zn porphyrin amphiphiles with a Co catalyst in water for CO2-to-methane conversion with a turnover number >6,600 and 89% selectivity over 30 days. The hierarchical self-assembly induced a spherical antenna effect that could facilitate the photocatalytic process with an initial 15% solar-to-fuel efficiency. Furthermore, it has a capability to efficiently reduce atmospheric CO2 into methane with high selectivity in water.