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利用空穴转移剂提高石墨相氮化碳的光催化析氢活性

Promoting Photocatalytic Hydrogen Evolution Activity of Graphitic Carbon Nitride with Hole-Transfer Agents.

作者信息

Indra Arindam, Beltrán-Suito Rodrigo, Müller Marco, Sivasankaran Ramesh P, Schwarze Michael, Acharjya Amitava, Pradhan Bapi, Hofkens Johan, Brückner Angelika, Thomas Arne, Menezes Prashanth W, Driess Matthias

机构信息

Department of Chemistry, Indian Institute of Technology, Banaras Hindu University, 221005, Varanasi, Uttar Pradesh, India.

Metalorganics and Inorganic Materials, Department of Chemistry, Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623, Berlin, Germany.

出版信息

ChemSusChem. 2021 Jan 7;14(1):306-312. doi: 10.1002/cssc.202002500. Epub 2020 Nov 27.

Abstract

Visible light-driven photocatalytic reduction of protons to H is considered a promising way of solar-to-chemical energy conversion. Effective transfer of the photogenerated electrons and holes to the surface of the photocatalyst by minimizing their recombination is essential for achieving a high photocatalytic activity. In general, a sacrificial electron donor is used as a hole scavenger to remove photogenerated holes from the valence band for the continuation of the photocatalytic hydrogen (H ) evolution process. Here, for the first time, the hole-transfer dynamics from Pt-loaded sol-gel-prepared graphitic carbon nitride (Pt-sg-CN) photocatalyst were investigated using different adsorbed hole acceptors along with a sacrificial agent (ascorbic acid). A significant increment (4.84 times) in H production was achieved by employing phenothiazine (PTZ) as the hole acceptor with continuous H production for 3 days. A detailed charge-transfer dynamic of the photocatalytic process in the presence of the hole acceptors was examined by time-resolved photoluminescence and in situ electron paramagnetic resonance studies.

摘要

可见光驱动的光催化将质子还原为氢气被认为是太阳能转化为化学能的一种很有前景的方式。通过最小化光生电子和空穴的复合,将它们有效地转移到光催化剂表面对于实现高光催化活性至关重要。一般来说,牺牲电子供体用作空穴清除剂,以从价带中去除光生空穴,从而延续光催化析氢(H₂)过程。在此,首次使用不同的吸附空穴受体以及牺牲剂(抗坏血酸)研究了负载铂的溶胶 - 凝胶制备的石墨相氮化碳(Pt - sg - CN)光催化剂的空穴转移动力学。通过使用吩噻嗪(PTZ)作为空穴受体,实现了氢气产量显著增加(4.84倍),并连续3天持续产氢。通过时间分辨光致发光和原位电子顺磁共振研究,研究了空穴受体存在下光催化过程的详细电荷转移动力学。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f378/7839742/e0af80bfedd1/CSSC-14-306-g001.jpg

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