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间隙磷掺杂和MoS修饰对ZnCdS光催化高效产氢的协同作用。

Synergistic effect of interstitial phosphorus doping and MoS modification over ZnCdS for efficient photocatalytic H production.

作者信息

Liu Qian, You Junhua, Xiong Ya, Liu Wendi, Song Mingfang, Ren Jiali, Xue Qingzhong, Tian Jian, Zhang Hangzhou, Wang Xiaoxue

机构信息

School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, Shandong, PR China.

School of Materials Science and Engineering, Shenyang University of Technology, Shenyang 110870, Liaoning, PR China.

出版信息

J Colloid Interface Sci. 2024 Dec;675:772-782. doi: 10.1016/j.jcis.2024.07.044. Epub 2024 Jul 6.

Abstract

ZnCdS photocatalysts have been widely investigated due to their diverse morphologies, suitable band gaps/band edge positions, and high electronic mobility. However, the sluggish charge separation and severe charge recombination impede the application of ZnCdS for hydrogen evolution reaction (HER). Herein, doping of phosphorus (P) atoms into ZnCdS has been implemented to elevate S vacancies concentration as well as tune its Fermi level to be located near the impurity level of S vacancies, prolonging the lifetime of photogenerated electrons. Moreover, P doping induces a hybridized state in the bandgap, leading to an imbalanced charge distribution and a localized built-in electric field for effective separation of photogenerated charge carriers. Further construction of intimate heterojunctions between P-ZnCdS and MoS accelerates surface redox reaction. Benefiting from the above merits, 1 % MoS/P-ZnCdS exhibits a high hydrogen production rate of 30.65 mmol·g·h with AQE of 22.22 % under monochromatic light at 370 nm, exceeding most ZnCdS based photocatalysts reported so far. This work opens avenues to fabricate examplary photocatalysts for solar energy conversion and beyond.

摘要

硫化锌镉(ZnCdS)光催化剂因其多样的形貌、合适的带隙/能带边缘位置以及高电子迁移率而受到广泛研究。然而,缓慢的电荷分离和严重的电荷复合阻碍了ZnCdS在析氢反应(HER)中的应用。在此,通过将磷(P)原子掺杂到ZnCdS中,提高了硫空位浓度,并将其费米能级调整到接近硫空位的杂质能级,从而延长了光生电子的寿命。此外,P掺杂在带隙中诱导出杂化态,导致电荷分布不平衡并产生局部内建电场,以有效分离光生电荷载流子。进一步在P-ZnCdS和MoS之间构建紧密的异质结加速了表面氧化还原反应。受益于上述优点,1%的MoS/P-ZnCdS在370nm单色光下表现出30.65mmol·g·h的高产氢率,量子效率为22.22%,超过了目前报道的大多数基于ZnCdS的光催化剂。这项工作为制备用于太阳能转换及其他领域的示范性光催化剂开辟了道路。

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