期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 11, 页码 3484-3497出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00088a
关键词
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资金
- Department of Science and Technology, DST-SERB, New Delhi, Govt. of India [CRG/2020/000244]
- Council of Scientific and Industrial Research, CSIR, New Delhi, Govt. of India [02(0453)/21/EMR-II]
- University of Kalyani
- DST, Govt. of India
A new triazine-based organized 2D covalent organic framework, TRITER-2, displayed excellent photocatalytic activity for the synthesis of methanol through the reduction of CO2. The material showed a high surface area and could be recycled multiple times without losing its catalytic performance. This sustainable and efficient catalyst offers a low-cost, non-toxic, and low carbon footprint route for the synthesis of methanol.
A new triazine-based organized 2D covalent organic framework (COF), namely, TRITER-2, was built through combinatorial copolymerization between 4,4 '-biphenyldicarbaldehyde and a triamine 1,3,5-tris-(4-aminophenyl) triazine (TAPT). This highly crystalline organic polymeric material displayed a superior BET surface area (1260 m(2) g(-1)) and exceptional photocatalytic activity for the synthesis of methanol. The metal-free catalytic reduction to methanol has emerged as a sustainable avenue due to the ambient reaction conditions by which CO2 is reduced to methanol. The catalytic reduction of CO2 under metal-free conditions offered the synthesis of methanol at a low price, in a non-toxic way with earth-abundant reagents, and a low carbon footprint. Using this COF TRITER-2, we have carried out the photocatalytic reduction of CO2 into high-value methanol as the active photo-catalyst under atmospheric pressure CO2. The highest turnover number (TON = 141) for visible-light-accelerated metal-free CO2 reduction to methanol (major product) using crystalline TRITER-2 (10 mg) was achieved under 20 W white LED irradiation. The reaction did not proceed without any applied potential (i.e., a white LED) and can be readily monitored by altering the light intensity. We demonstrate that a TON of about 10 can be reached with sunlight under sustainable reaction conditions. This catalyst is efficient, selective, and can be recycled several times, retaining its catalytic performance.
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