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Synergy of yolk-shelled structure and tunable oxygen defect over CdS/CdCO3-CoS2: Wide band-gap semiconductors assist in efficient visible-light-driven H2 production and CO2 reduction
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2022-11-02 , DOI: 10.1016/j.cej.2022.140113
Siyi Zhang , Shiwen Du , Yumin Wang , Ziwu Han , Xu Li , Guojun Li , Qing Hu , Hu Xu , Chunqing He , Pengfei Fang

Yolk-shelled CoS2 nanospheres are designed through Kirkendall Effect and subsequently converted into defect-rich CdS/CdCO3-CoS2 photocatalysts via in-situ growth method. The optimal CdS/CdCO3-CoS2 exhibits a significant hydrogen evolution rate of 64867.88 μmol h-1 gcat-1 that is 3.23 and 49.45 folds higher than CoS2-CdS and pure CdS. CO2 reduction rate of CdS/CdCO3-CoS2 is detected additionally (654.7 μmol h-1 gcat-1). Yolk-shelled CdS/CdCO3-CoS2 induces the multi-scattering of incident light, possessing 1.52-fold H2 production rate than that of full hollow ones. Enhanced photoexcited-carriers migration efficiency is attributed to the synergistic effect between possible Mie resonance at about λ = 450 nm in yolk-shelled architecture based on Mie’s theory and monochromatic light HER test, and the formation of defect energy level within the wide-band gap of CdCO3 in Schottky-type/type II heterojunction. Electron paramagnetic resonance, positron annihilation spectroscopy and density functional theory calculation etc. are employed to validate the presence of oxygen vacancies and the photocatalytic mechanism.



中文翻译:

蛋黄壳结构和 CdS/CdCO3-CoS2 上的可调谐氧缺陷的协同作用:宽带隙半导体有助于有效的可见光驱动 H2 生产和 CO2 减少

蛋黄壳CoS 2纳米球是通过柯肯达尔效应设计的,随后通过原位生长方法转化为富含缺陷的CdS/CdCO 3 -CoS 2光催化剂。最佳CdS/CdCO 3 -CoS 2的析氢速率显着为64867.88 μmol h -1 g cat -1 ,分别是CoS 2 -CdS和纯CdS的3.23倍和49.45倍。另外检测CdS/CdCO 3 -CoS 2的CO 2还原率(654.7 μmol h -1 g cat -1 )。蛋黄壳 CdS/CdCO 3 -CoS2引起入射光的多次散射,H 2的产生率是全空心的1.52倍。增强的光激发载流子迁移效率归因于基于 Mie 理论的蛋黄壳结构中约 λ = 450 nm 处可能的 Mie 共振和单色光 HER 测试之间的协同效应,以及在宽带隙内形成缺陷能级肖特基型/II型异质结中的CdCO 3 。采用电子顺磁共振、正电子湮没光谱和密度泛函理论计算等方法验证了氧空位的存在和光催化机理。

更新日期:2022-11-05
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