| Autor: |
Das R; New Chemistry Unit and School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore560064, India.; School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore560064, India., Paul R; Department of Catalysis & Fine Chemicals, CSIR-Indian Institute of Chemical Technology, Uppal Road, Hyderabad500007, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad201002, India., Parui A; Materials Research Centre, Indian Institute of Science, Bangalore560012, India., Shrotri A; Institute for Catalysis, Hokkaido University, Kita 21 Nishi 10, Kita-Ku, Sapporo001-0021, Japan., Atzori C; European Synchrotron Radiation Facility, 71 Avenue des Martyrs, CS 40220, 38043Grenoble Cedex 9, France., Lomachenko KA; European Synchrotron Radiation Facility, 71 Avenue des Martyrs, CS 40220, 38043Grenoble Cedex 9, France., Singh AK; Materials Research Centre, Indian Institute of Science, Bangalore560012, India., Mondal J; Department of Catalysis & Fine Chemicals, CSIR-Indian Institute of Chemical Technology, Uppal Road, Hyderabad500007, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad201002, India., Peter SC; New Chemistry Unit and School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore560064, India.; School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore560064, India. |
| Abstrakt: |
The development of an efficient photocatalyst for C2 product formation from CO 2 is of urgent importance toward the deployment of solar-fuel production. Here, we report a template-free, cost-effective synthetic strategy to develop a carbazole-derived porous organic polymer (POP)-based composite catalyst. The composite catalyst is comprised of In 2.77 S 4 and porous organic polymer (POP) and is held together by induced-polarity-driven electrostatic interaction. Utilizing the synergy of the catalytically active In centers and light-harvesting POPs, the catalyst showed 98.9% selectivity toward the generation of C 2 H 4 , with a formation rate of 67.65 μmol g -1 h -1 . Two different oxidation states of the In 2.77 S 4 spinel were exploited for the C-C coupling process, and this was investigated by X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and density functional theory (DFT) calculations. The role of POP was elucidated via several photophysical and photoelectrochemical studies. The electron transfer was mapped by several correlated approaches, which assisted in establishing the Z-scheme mechanism. Furthermore, the mechanism of C 2 H 4 formation was extensively investigated using density functional theory (DFT) calculations from multiple possible pathways. |
