金属硒化物用于以石墨烯为电子介质的光催化Z机制全分解水体系

doi:10.1016/S1872-2067(19)63326-7

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1668-1672.DOI: 10.1016/S1872-2067(19)63326-7

金属硒化物用于以石墨烯为电子介质的光催化Z机制全分解水体系

陈闪山^a, 久富隆史^a, 马贵军^b, 王征^a, 潘振华^b, 高田刚^a, 堂免一成^a,b

a 信州大学能源与环境科学中心, 长野 3808553, 日本;
b 东京大学工学院, 东京 1138656, 日本

收稿日期:2019-01-22 修回日期:2019-02-17 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: 堂免一成
基金资助:
This work was financially supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization (NEDO) and Grant-in-Aids for Scientific Research (A) (No. 16H02417) and Young Scientists (A) (No. 15H05494) from the Japan Society for the Promotion of Science (JSPS).

Metal selenides for photocatalytic Z-scheme pure water splitting mediated by reduced graphene oxide

Shanshan Chen^a, Takashi Hisatomi^a, Guijun Ma^b, Zheng Wang^a, Zhenhua Pan^b, Tsuyoshi Takata^a, Kazunari Domen^a,b

a Center for Energy & Environmental Science, Shinshu University, 4-17-1 Wakasato, Nagano-shi, Nagano 380-8553, Japan;
b Department of Chemical System Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

Received:2019-01-22 Revised:2019-02-17 Online:2019-11-18 Published:2019-09-06
Supported by:
This work was financially supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization (NEDO) and Grant-in-Aids for Scientific Research (A) (No. 16H02417) and Young Scientists (A) (No. 15H05494) from the Japan Society for the Promotion of Science (JSPS).

摘要/Abstract

摘要： 基于粉末半导体催化剂的太阳能光催化分解水技术因具有廉价和适宜大规模生产等优点正日益成为未来重要的制氢技术之一.开发高效光催化分解水体系的一个重要前提是使用窄带隙半导体材料，从而能最大化地吸收和利用太阳光谱.近年来，一些诸如氮（氧）化物、硫（氧）化物和硒化物等窄带隙半导体材料陆续被开发和拓展到光催化全分解水体系中.然而，考虑到随着吸收波长的提高而导致氧化还原反应驱动力减小的挑战，开发基于窄带隙半导体催化剂的高效全分解水体系依然是当今光催化研究领域的主题之一.
金属硒化物作为一类窄带隙半导体材料，较同类氧化物和硫化物具有更长的吸收带边.前期我们课题组利用金层锚定的硒化锌和铜镓硒固溶体（ZnSe：CGSe）产氢催化剂与CoO_x/BiVO₄产氧催化剂组合实现了首例基于硒化物的可见光驱动Z机制全分解纯水.为了进一步探索更多基于硒化物构筑Z机制全分解水催化体系的可能，本文通过调变Zn/（Zn+Cu）和Ga/Cu摩尔比制备了吸收带边在480-730 nm范围内可调的系列ZnSe：CGSe样品，并以此硒化物为产氢催化剂，结合CoO_x/BiVO₄产氧催化剂以及还原石墨烯（RGO）电子介质成功构筑了另一种Z机制全分解纯水催化体系.该体系与前期报道的体系相比，避免了真空蒸镀工艺过程，构筑起来更为简单便捷.研究表明，光催化分解水效率与对应硒化物光阴极的光电性能密切相关，而与有牺牲试剂存在下的硒化物产氢活性不呈线性关系.

关键词: 产氢, 光催化, 硒化物, 水分解, Z机制

Abstract: Exploration of novel narrow bandgap semiconductors for overall water splitting is vital for the realization of practical solar H₂ production. In the work, solid solutions of zinc selenide and copper gallium selenide with absorption edge wavelengths ranging from 480 to 730 nm were developed. Using these metal selenides as H₂-evolving photocatalysts, CoO_x/BiVO₄ as the O₂-evolving photocatalyst, and reduced graphene oxide as the electron mediator, all-solid-state Z-scheme overall pure water splitting systems were constructed. The rate of photocatalytic H₂ evolution from aqueous solutions containing Na₂S and Na₂SO₃ as the electron donors was evaluated while employing these selenide photocatalysts at various Zn/(Zn+Cu) and Ga/Cu molar ratios. The data demonstrate that efficient Z-scheme overall water splitting was significantly correlated to the photoelectrochemical performance of the selenide photocatalysts acting as photocathodes, rather than the photocatalytic activities of these materials during the sacrificial H₂ evolution.

Key words: Hydrogen production, Photocatalysis, Selenide, Water splitting, Z-scheme

陈闪山, 久富隆史, 马贵军, 王征, 潘振华, 高田刚, 堂免一成. 金属硒化物用于以石墨烯为电子介质的光催化Z机制全分解水体系[J]. 催化学报, 2019, 40(11): 1668-1672.

Shanshan Chen, Takashi Hisatomi, Guijun Ma, Zheng Wang, Zhenhua Pan, Tsuyoshi Takata, Kazunari Domen. Metal selenides for photocatalytic Z-scheme pure water splitting mediated by reduced graphene oxide[J]. Chinese Journal of Catalysis, 2019, 40(11): 1668-1672.

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金属硒化物用于以石墨烯为电子介质的光催化Z机制全分解水体系

Metal selenides for photocatalytic Z-scheme pure water splitting mediated by reduced graphene oxide

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