An antimonene/Cp*Rh(phen)Cl/black phosphorus hybrid nanosheet-based Z-scheme artificial photosynthesis for enhanced photo/bio-catalytic CO2 reduction. Issue 1 (6th December 2019)

• Record Type: Journal Article
• Authors: Ji, Xiaoyuan; Kang, Yong; Fan, Taojian; Xiong, Qingqing; Zhang, Songping; Tao, Wei; Zhang, Han
• Is Part Of: Journal of materials chemistry. Volume 8:Issue 1(2020)
• Page Start: 323
• Page End: 333
• Publication Date: 2019-12-06
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/c9ta11167k
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : A biomimicking Z-scheme photocatalytic system was constructed using dual-functionalized polymer covalent cross-linking electron mediator to catenate antimonene and black phosphorus nanosheets. Abstract : Developing a biocatalyzed artificial photosynthesis system (APS) with a Z-scheme for CO2 conversion has a promising outlook. However, it remains unexplored and challenging. Herein, we present an antimonene (AM) and black phosphorus (BP) hybrid nanosheet (HNSs) based Z-scheme APS for enhanced photo/bio-catalytic CO2 reduction. An "amphipathic" polymer PEI-PEG-C18 with a positively charged PEI-head and hydrophobic C18-tail was synthesized and further modified with an electron mediator (M, Cp*Rh(phen)Cl). Using this PEI-PEG-C18-M as a "double-side tap", AM/M/BP HNS-based Z-scheme photocatalytic systems were constructed through catenating AM NSs via a hydrophobic interaction with the hydrophobic C18-tail and subsequent BP NSs via electrostatic interactions with the positively charged PEI-head. Thereafter, the biocatalytic system, including NAD(H) + and redox enzymes, were sandwiched between the AM and BP layers through an electrostatic attraction with the amide groups in the "double-side tap". Due to the high separation efficiency of the photogenerated electrons and holes and the improved reduction and oxidation potentials, the integrated Z-scheme APS shows excellent performance. In particular, although neither AM nor BP could catalyze NADH regeneration using H2 O as an electron donor under visible light, a 35 ± 4% regeneration of NADH and 160 ± 24 μmol formic acid production were achieved by the AM/M/BP HNS-based Z-scheme APS. Moreover, the compatibility and omnipotence of the HNS-based APS for the synthesis of other high value-added products from CO2 have been demonstrated through assembling the corresponding biocatalysts.