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Rhenium-modified porous covalent triazine framework for highly efficient photocatalytic carbon dioxide reduction in a solid–gas system†‡
Catalysis Science & Technology ( IF 5 ) Pub Date : 2018-03-19 00:00:00 , DOI: 10.1039/c8cy00176f
Rui Xu 1, 2, 3, 4, 5 , Xu-Sheng Wang 1, 2, 3, 4, 5 , Hui Zhao 1, 2, 3, 4, 5 , Hua Lin 1, 2, 3, 4, 5 , Yuan-Biao Huang 1, 2, 3, 4, 5 , Rong Cao 1, 2, 3, 4, 5
Affiliation  

The conversion of CO2 into valuable chemicals by means of solar energy with high efficiency is a promising alternative for decreasing greenhouse gas and solving the energy shortage. Porous covalent triazine frameworks (CTFs) have attracted considerable attention in gas adsorption and heterogeneous catalysis owing to their abundant nitrogen sites and very high thermal, chemical, and mechanical stability. In this work, a pyridine-based CTF (CTF-py, py = pyridine) derived from 2,6-dicyanopyridine is employed as a porous platform to anchor the Re carbonyl complex Re(CO)3Cl (Re-CTF-py), which exhibits high efficiency in the photocatalytic CO2 reduction to CO with a turnover number (TON) of 4.8; the CO evolution rate for Re-CTF-py reached 353.05 μmol g−1 h−1 within 10 hours under full light irradiation in a solid–gas system. Moreover, in the solid–gas system, the single-site Re-CTF-py catalyst could prevent Re active species dimerization and leaching that lead to deactivation. This work highlights the great potential of using stable CTFs as porous platforms to anchor single active sites for heterogeneous catalysis.

中文翻译:

hen修饰的多孔共价三嗪骨架,可在固-气系统中高效还原光催化二氧化碳

通过太阳能将CO 2高效转化为有价值的化学物质是减少温室气体和解决能源短缺的有前途的替代方法。多孔共价三嗪骨架(CTF)由于其丰富的氮位以及非常高的热,化学和机械稳定性而在气体吸附和非均相催化方面引起了相当大的关注。在这项工作中,衍生自2,6-二氰基吡啶的吡啶基CTF(CTF-py,py =吡啶)被用作固定Re羰基配合物Re(CO)3 Cl(Re-CTF-py)的多孔平台。,其在将CO 2光催化还原为CO方面表现出高效率,周转数(TON)为4.8;Re-CTF-py的CO释放速率达到353.05μmolg在固态气体系统中,在全光照射下10小时内-1 h -1。此外,在固-气系统中,单中心的Re-CTF-py催化剂可以防止Re活性物质二聚和浸出,从而导致失活。这项工作凸显了使用稳定的CTF作为多孔平台锚定单个活性位进行多相催化的巨大潜力。
更新日期:2018-03-19
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