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光催化填充床流动反应器中液态有机载体的室温连续氢释放

Continuous Room-Temperature Hydrogen Release from Liquid Organic Carriers in a Photocatalytic Packed-Bed Flow Reactor.

作者信息

Ibrahim Malek Y S, Bennett Jeffrey A, Abolhasani Milad

机构信息

Department of Chemical and Biomolecular Engineering, North Carolina State University, 911 Partners Way, Raleigh, NC 27695, USA.

出版信息

ChemSusChem. 2022 Jul 21;15(14):e202200733. doi: 10.1002/cssc.202200733. Epub 2022 May 18.

DOI:10.1002/cssc.202200733
PMID:35446510
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9400973/
Abstract

Despite the potential of hydrogen (H ) storage in liquid organic carriers to achieve carbon neutrality, the energy required for H release and the cost of catalyst recycling have hindered its large-scale adoption. In response, a photo flow reactor packed with rhodium (Rh)/titania (TiO ) photocatalyst was reported for the continuous and selective acceptorless dehydrogenation of 1,2,3,4-tetrahydroquinoline to H gas and quinoline under visible light irradiation at room temperature. The tradeoff between the reactor pressure drop and its photocatalytic surface area was resolved by selective in-situ photodeposition of Rh in the photo flow reactor post-packing on the outer surface of the TiO microparticles available to photon flux, thereby reducing the optimal Rh loading by 10 times compared to a batch reactor, while facilitating catalyst reuse and regeneration. An example of using quinoline as a hydrogen acceptor to lower the energy of the hydrogen production step was demonstrated via the water-gas shift reaction.

摘要

尽管在液态有机载体中储存氢有实现碳中和的潜力，但释放氢所需的能量和催化剂回收成本阻碍了其大规模应用。作为回应，有报道称一种装有铑（Rh）/二氧化钛（TiO₂）光催化剂的光流反应器，可在室温可见光照射下将1,2,3,4 - 四氢喹啉连续且选择性地进行无受体脱氢反应生成氢气和喹啉。通过在光流反应器装填后，在可被光子通量照射到的TiO₂微粒外表面选择性地原位光沉积Rh，解决了反应器压降与其光催化表面积之间的权衡问题，从而使最佳Rh负载量比间歇式反应器降低了10倍，同时便于催化剂的重复使用和再生。通过水煤气变换反应展示了一个使用喹啉作为氢受体来降低制氢步骤能量的例子。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/a01aa4294d2d/CSSC-15-0-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/cb29bd1dbc4a/CSSC-15-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/84edd63a62a0/CSSC-15-0-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/98ccbb826ac7/CSSC-15-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/157fef791555/CSSC-15-0-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/b0eb99ce567a/CSSC-15-0-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/a01aa4294d2d/CSSC-15-0-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/cb29bd1dbc4a/CSSC-15-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/84edd63a62a0/CSSC-15-0-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/98ccbb826ac7/CSSC-15-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/157fef791555/CSSC-15-0-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/b0eb99ce567a/CSSC-15-0-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ca/9400973/a01aa4294d2d/CSSC-15-0-g004.jpg

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