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具有Co-S键的高效、全光谱驱动的H演化Z型CoP/CdS光催化剂。

Efficient, Full Spectrum-Driven H Evolution Z-Scheme CoP/CdS Photocatalysts with Co-S Bonds.

作者信息

Li Nan, Ding Yunxuan, Wu Jiaojiao, Zhao Zhijie, Li Xitao, Zheng Yan-Zhen, Huang Meilan, Tao Xia

机构信息

School of Chemistry & Chemical Engineering , Queen's University Belfast , Belfast BT9 5AG , U.K.

出版信息

ACS Appl Mater Interfaces. 2019 Jun 26;11(25):22297-22306. doi: 10.1021/acsami.9b03965. Epub 2019 Jun 17.

Abstract

Exploring high-efficiency, low-cost, and stable photocatalysts that enable full solar spectrum including UV, visible, and near-infrared (NIR) light utilization for photocatalytic hydrogen generation still faces huge challenge. Herein, a CoP/CdS Z-scheme photocatalyst without a noble metal is rationally fabricated to achieve ultrabroad UV-vis-NIR harvesting. Compared to Pt/CdS, CdS, and CoP, the optimized CoP/CdS exhibits much more outstanding performance with the H generation rates of 262.16, 66.98, and 3.93 mmol/g/h under solar, visible (780 nm > λ > 420 nm), and NIR (λ > 780 nm) light, respectively. Particularly, 10% CoP/CdS displays a prominent apparent quantum efficiency value of 2.26% at 700 nm. The Z-scheme transform route can effectively enhance the separation of charge carriers in CoP/CdS for UV-vis-driven HER, as confirmed by photoluminescence and photoelectrochemical measurements. More importantly, the Co-S bonds at the interface demonstrated by Fourier transform infrared, Raman (mapping), and X-ray photoelectron spectroscopy and density functional theory calculations can act as a "bridge" for charge transfer, thereby enhancing the full spectrum-driven H evolution. To the best of our knowledge, this is a rare research on full spectrum-driven photocatalytic HER without a noble metal.

摘要

探索能够实现包括紫外线、可见光和近红外(NIR)光在内的全太阳光谱利用以进行光催化产氢的高效、低成本且稳定的光催化剂仍然面临巨大挑战。在此,一种不含贵金属的CoP/CdS Z型光催化剂被合理制备以实现超宽的紫外-可见-近红外光捕获。与Pt/CdS、CdS和CoP相比,优化后的CoP/CdS表现出更为出色的性能,在太阳光、可见光(780 nm>λ>420 nm)和近红外光(λ>780 nm)下的产氢速率分别为262.16、66.98和3.93 mmol/g/h。特别地,10% CoP/CdS在700 nm处显示出2.26%的显著表观量子效率值。光致发光和光电化学测量证实,Z型转换途径可以有效增强CoP/CdS中电荷载流子的分离以用于紫外-可见光驱动的析氢反应。更重要的是,傅里叶变换红外光谱、拉曼(映射)光谱、X射线光电子能谱和密度泛函理论计算表明,界面处的Co-S键可以作为电荷转移的“桥梁”,从而增强全光谱驱动的析氢反应。据我们所知,这是一项罕见的关于无贵金属全光谱驱动光催化析氢反应的研究。

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