Affiliation:
1. Chemistry and Physics of Materials Unit (CPMU) School of Advanced Materials (SAMat) International Centre for Materials Science (ICMS) Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR) 560064 Jakkur Bangalore India
2. New Chemistry Unit (NCU) School of Advanced Materials (SAMat) International Centre for Materials Science (ICMS) Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR) 560064 Jakkur Bangalore India
Abstract
AbstractEfficient solar‐driven syngas production (CO+H2 mixture) from CO2 and H2O with a suitable photocatalyst and fundamental understanding of the reaction mechanism are the desired approach towards the carbon recycling process. Herein, we report the design and development of an unique COF‐topological quantum material nano‐heterostructure, COF@TI with a newly synthesized donor‐acceptor based COF and two dimensional (2D) nanosheets of strong topological insulator (TI), PbBi2Te4. The intrinsic robust metallic surfaces of the TI act as electron reservoir, minimising the fast electron‐hole recombination process, and the presence of 6s2 lone pairs in Pb2+ and Bi3+ in the TI helps for efficient CO2 binding, which are responsible for boosting overall catalytic activity. In variable ratio of acetonitrile‐water (MeCN : H2O) solvent mixture COF@TI produces syngas with different ratios of CO and H2. COF@TI nano‐heterostructure enables to produce higher amount of syngas with more controllable ratios of CO and H2 compared to pristine COF. The electron transfer route from COF to TI was realized from Kelvin probe force microscopy (KPFM) analysis, charge density difference calculation, excited state lifetime and photoelectrochemical measurements. Finally, a probable mechanistic pathway has been established after identifying the catalytic sites and reaction intermediates by in situ DRIFTS study and DFT calculation.