Fabrication of Low Adsorption Energy Ni-Mo Cluster Cocatalyst in Metal-Organic Frameworks for Visible Photocatalytic Hydrogen Evolution | |
Department | OSSO国家重点实验室 |
Zhen WL(甄文龙)1,2; Gao, Haibo1,2; Tian B(田彬)1; Ma JT(马建泰)2; Lu GX(吕功煊)1,2; Lv GX(吕功煊) | |
2016 | |
Source Publication | ACS Applied Materials and Interfaces |
ISSN | 1944-8244 |
Volume | 8Issue:17Pages:10808-10819 |
Abstract | An effective cocatalyst is crucial for enhancing the visible photocatalytic performance of the hydrogen generation reaction. By using density-functional theory (DFT) and frontier molecular orbital (FMO) theory calculation analysis, the hydrogen adsorption free energy (ΔGH) of Ni–Mo alloy (458 kJ·mol–1) is found to be lower than that of Ni itself (537 kJ·mol–1). Inspired by these results, the novel, highly efficient cocatalyst NiMo@MIL-101 for photocatalysis of the hydrogen evolution reaction (HER) was fabricated using the double solvents method (DSM). In contrast with Ni@MIL-101 and Mo@MIL-101, NiMo@MIL-101 exhibited an excellent photocatalytic performance (740.2 μmol·h–1 for HER), stability, and high apparent quantum efficiency (75.7%) under 520 nm illumination at pH 7. The NiMo@MIL-101 catalyst also showed a higher transient photocurrent, lower overpotential (−0.51 V), and longer fluorescence lifetime (1.57 ns). The results uncover the dependence of the photocatalytic activity of HER on the ΔGH of Ni–Mo (MoNi4) alloy nanoclusters, i.e., lower ΔGH corresponding to higher HER activity for the first time. The NiMo@MIL-101 catalyst could be a promising candidate to replace precious-metal catalysts of the HER. |
Keyword | Nimo@mil-101 Density Functional Theory Low Adsorption Energy Visible Photocatalytic Hydrogen Generation Apparent Quantum Efficiency |
Subject Area | 物理化学与绿色催化 |
DOI | 10.1021/acsami.5b12524 |
Funding Organization | the NSFC (Grant Nos. 21373245;21433007);973 Program of China (No. 2013CB632404) |
Indexed By | SCI |
If | 7.504 |
Language | 英语 |
Funding Project | 环境催化与清洁能源研究组 |
compositor | 第一作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/20091 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Lv GX(吕功煊) |
Affiliation | 1.Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China 2.Lanzhou Univ, Coll Chem & Chem Engn, Lanzhou 730000, Peoples R China |
Recommended Citation GB/T 7714 | Zhen WL,Gao, Haibo,Tian B,et al. Fabrication of Low Adsorption Energy Ni-Mo Cluster Cocatalyst in Metal-Organic Frameworks for Visible Photocatalytic Hydrogen Evolution[J]. ACS Applied Materials and Interfaces,2016,8(17):10808-10819. |
APA | Zhen WL,Gao, Haibo,Tian B,Ma JT,Lu GX,&吕功煊.(2016).Fabrication of Low Adsorption Energy Ni-Mo Cluster Cocatalyst in Metal-Organic Frameworks for Visible Photocatalytic Hydrogen Evolution.ACS Applied Materials and Interfaces,8(17),10808-10819. |
MLA | Zhen WL,et al."Fabrication of Low Adsorption Energy Ni-Mo Cluster Cocatalyst in Metal-Organic Frameworks for Visible Photocatalytic Hydrogen Evolution".ACS Applied Materials and Interfaces 8.17(2016):10808-10819. |
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