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用于高效可见光驱动析氢和析氧的具有增强电荷载流子分离性能的Co(OH)/ZnCr层状双氢氧化物“p-n”异质结光催化剂的制备

Fabrication of a Co(OH)/ZnCr LDH "p-n" Heterojunction Photocatalyst with Enhanced Separation of Charge Carriers for Efficient Visible-Light-Driven H and O Evolution.

作者信息

Sahoo Dipti Prava, Nayak Susanginee, Reddy K Hemalata, Martha Satyabadi, Parida Kulamani

机构信息

Centre for Nanoscience and Technology , Siksha 'O' Anusandhan (Deemed to be) University , Bhubaneswar 751030 , India.

出版信息

Inorg Chem. 2018 Apr 2;57(7):3840-3854. doi: 10.1021/acs.inorgchem.7b03213. Epub 2018 Mar 12.

Abstract

Photocatalytic generation of H and O by water splitting remains a great challenge for clean and sustainable energy. Taking into the consideration promising heterojunction photocatalysts, analogous energy issues have been mitigated to a meaningful extent. Herein, we have architectured a highly efficient bifunctional heterojunction material, i.e., p-type Co(OH) platelets with an n-type ZnCr layered double hydroxide (LDH) by an ultrasonication method. Primarily, the Mott-Schottky measurements confirmed the n- and p-type semiconductive properties of LDH and CH material, respectively, with the construction of a p-n heterojunction. The high resolution transmission electron microscopy results suggest that surface modification of ZnCr LDH by Co(OH) hexagonal platelets could form a fabulous p-n interfacial region that significantly decreases the energy barrier for O and H production by effectively separating and transporting photoinduced charge carriers, leading to enhanced photoreactivity. A deep investigation into the mechanism shows that a 30 wt % Co(OH)-modified ZnCr LDH sample liberates maximum H and O production in 2 h, i.e., 1115 and 560 μmol, with apparent conversion efficiencies of H and O evolution of 13.12% and 6.25%, respectively. Remarkable photocatalytic activity with energetic charge pair transfer capability was illustrated by electrochemical impedance spectroscopy, linear sweep voltammetry, and photoluminescence spectra. The present study clearly suggests that low-cost Co(OH) platelets are the most crucial semiconductors to provide a new p-n heterojunction photocatalyst for photocatalytic H and O production on the platform of ZnCr LDH.

摘要

通过水分解光催化生成氢气和氧气仍然是清洁和可持续能源面临的巨大挑战。考虑到有前景的异质结光催化剂,类似的能源问题已在一定程度上得到缓解。在此,我们通过超声法构建了一种高效的双功能异质结材料,即具有n型ZnCr层状双氢氧化物(LDH)的p型Co(OH)片状物。首先,莫特-肖特基测量分别证实了LDH和CH材料的n型和p型半导体性质,并构建了p-n异质结。高分辨率透射电子显微镜结果表明,Co(OH)六方片状物对ZnCr LDH的表面改性可以形成一个极好的p-n界面区域,通过有效地分离和传输光生电荷载流子,显著降低了氢气和氧气生成的能垒,从而提高了光反应活性。对机理的深入研究表明,30 wt% Co(OH)改性的ZnCr LDH样品在2小时内释放出最大的氢气和氧气产量,即分别为1115和560 μmol,氢气和氧气析出的表观转换效率分别为13.12%和6.25%。电化学阻抗谱、线性扫描伏安法和光致发光光谱表明了该材料具有显著的光催化活性和高能电荷对转移能力。本研究清楚地表明,低成本的Co(OH)片状物是在ZnCr LDH平台上提供用于光催化氢气和氧气生成的新型p-n异质结光催化剂的最关键半导体。

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