All the catalytic active sites of MoS2 for hydrogen evolution

Li, Guoqing; Zhang, Du; Qiao, Qiao; Yu, Yifei; Peterson, David; Zafar, Abdullah; Kumar, Raj; Curtarolo, Stefano; Hunte, Frank; Shannon, Steve; Zhu, Yimei; Yang, Weitao; Cao, Linyou

doi:10.1021/jacs.6b05940

Title: All the catalytic active sites of MoS₂ for hydrogen evolution

Journal Article · Tue Nov 29 00:00:00 EST 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b05940· OSTI ID:1347369

Li, Guoqing ^[1]; Zhang, Du ^[2];

^[3]; Yu, Yifei ^[1];

^[1]; Zafar, Abdullah ^[1];

^[1]; Curtarolo, Stefano ^[2]; Hunte, Frank ^[1]; Shannon, Steve ^[1]; Zhu, Yimei ^[3]; Yang, Weitao ^[2];

^[1]

North Carolina State Univ., Raleigh, NC (United States)
Duke Univ., Durham, NC (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

MoS₂ presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS₂, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. Here, the intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s^–1 (65–75 mV/dec), 3.2 s^–1 (65–85 mV/dec), and 0.1 s^–1 (120–160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7–10%, and the number of sulfur vacancies in high crystalline quality MoS₂ is higher than that in low crystalline quality MoS₂, which may be related with the proximity of different local crystalline structures to the vacancies.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1347369

Report Number(s):: BNL-113649-2017-JA; R&D Project: MA015MACA; KC0201010

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 51; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 552 works

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Group 6 transition metal dichalcogenide nanomaterials: synthesis, applications and future perspectives Samadi, Morasae; Sarikhani, Navid; Zirak, Mohammad Nanoscale Horizons, Vol. 3, Issue 2 https://doi.org/10.1039/c7nh00137a	journal	January 2018
Distinctive optoelectronic properties of nanostructured ${MoS}_{2}$ bilayers Mlinar, Vladan Physical Review B, Vol. 100, Issue 8 https://doi.org/10.1103/physrevb.100.085411	journal	August 2019
Hydrogen evolution catalysis by molybdenum sulfides (MoS _x ): are thiomolybdate clusters like [Mo ₃ S ₁₃ ] ²⁻ suitable active site models? Grutza, Marie-Luise; Rajagopal, Ashwene; Streb, Carsten Sustainable Energy & Fuels, Vol. 2, Issue 9 https://doi.org/10.1039/c8se00155c	journal	January 2018
Using ligands to control reactivity, size and phase in the colloidal synthesis of WSe ₂ nanocrystals Geisenhoff, Jessica Q.; Tamura, Ashley K.; Schimpf, Alina M. Chemical Communications, Vol. 55, Issue 60 https://doi.org/10.1039/c9cc03326b	journal	January 2019
One-pot synthesis of manganese oxides and cobalt phosphides nanohybrids with abundant heterointerfaces in an amorphous matrix for efficient hydrogen evolution in alkaline solution Zhou, Dan; Wang, Zheng; Long, Xia Journal of Materials Chemistry A, Vol. 7, Issue 39 https://doi.org/10.1039/c9ta07601h	journal	January 2019
Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution Huang, Yichao; Sun, Yuanhui; Zheng, Xueli Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08877-9	journal	February 2019
Confined Catalysis: Progress and Prospects in Energy Conversion Shifa, Tofik Ahmed; Vomiero, Alberto Advanced Energy Materials, Vol. 9, Issue 40 https://doi.org/10.1002/aenm.201902307	journal	September 2019
Unveiling Active Sites for the Hydrogen Evolution Reaction on Monolayer MoS ₂ Zhang, Jing; Wu, Jingjie; Guo, Hua Advanced Materials, Vol. 29, Issue 42 https://doi.org/10.1002/adma.201701955	journal	September 2017
Activating MoS ₂ basal planes for hydrogen evolution through direct CVD morphology control Dong, Lianqing; Guo, Shaoqiang; Wang, Yuyan Journal of Materials Chemistry A, Vol. 7, Issue 48 https://doi.org/10.1039/c9ta08738a	journal	January 2019
Hydrogen interaction with selectively desulfurized MoS ₂ surface using Ne ⁺ sputtering Han, Sang Wook; Cha, Gi-Beom; Kang, Manil Journal of Applied Physics, Vol. 125, Issue 8 https://doi.org/10.1063/1.5079281	journal	February 2019
The Holy Grail in Platinum‐Free Electrocatalytic Hydrogen Evolution: Molybdenum‐Based Catalysts and Recent Advances Zhuang, Zechao; Huang, Jiazhao; Li, Yong ChemElectroChem, Vol. 6, Issue 14 https://doi.org/10.1002/celc.201900143	journal	June 2019
Hydrogen Evolution and Oxidation: Mechanistic Studies and Material Advances Tian, Xiaoyu; Zhao, Pengcheng; Sheng, Wenchao Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201808066	journal	December 2018
Surface Engineering of MoS ₂ via Laser‐Induced Exfoliation in Protic Solvents Gao, Zhi‐Wen; Liu, Mengjie; Zheng, Weiran Small, Vol. 15, Issue 44 https://doi.org/10.1002/smll.201903791	journal	September 2019
Vertically conductive MoS ₂ pyramids with a high density of active edge sites for efficient hydrogen evolution Zhou, Qingwei; Su, Shaoqiang; Cheng, Pengfei Journal of Materials Chemistry C, Vol. 8, Issue 9 https://doi.org/10.1039/c9tc05872a	journal	January 2020
Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution Luo, Zhaoyan; Ouyang, Yixin; Zhang, Hao Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04501-4	journal	May 2018
Understanding the unorthodox stabilization of liquid phase exfoliated molybdenum disulfide (MoS ₂ ) in water medium Rodriguez, Camila L. C.; Muñoz, Pablo A. R.; Donato, Katarzyna Z. Physical Chemistry Chemical Physics, Vol. 22, Issue 3 https://doi.org/10.1039/c9cp06422b	journal	January 2020
Electrochemical maps and movies of the hydrogen evolution reaction on natural crystals of molybdenite (MoS ₂ ): basal vs. edge plane activity Bentley, Cameron L.; Kang, Minkyung; Maddar, Faduma M. Chemical Science, Vol. 8, Issue 9 https://doi.org/10.1039/c7sc02545a	journal	January 2017
Atomic-Level Coupled Interfaces and Lattice Distortion on CuS/NiS ₂ Nanocrystals Boost Oxygen Catalysis for Flexible Zn-Air Batteries An, Li; Li, Yuxuan; Luo, Mingchuan Advanced Functional Materials, Vol. 27, Issue 42 https://doi.org/10.1002/adfm.201703779	journal	September 2017
1% defect enriches MoS ₂ quantum dot: catalysis and blue luminescence Tang, Jingmin; Sakamoto, Masanori; Ohta, Haruhisa Nanoscale, Vol. 12, Issue 7 https://doi.org/10.1039/c9nr07612c	journal	January 2020
Multi-layered photocathodes based on Cu ₂ ZnSnSe ₄ absorber and MoS ₂ catalyst for the hydrogen evolution reaction Grau, Sergi; Giraldo, Sergio; Saucedo, Edgardo Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/c9ta08818k	journal	January 2019
Insertion of Platinum Nanoparticles into MoS2 Nanoflakes for Enhanced Hydrogen Evolution Reaction Li, Dan; Li, Yang; Zhang, Bowei Materials, Vol. 11, Issue 9 https://doi.org/10.3390/ma11091520	journal	August 2018
Microwave-assisted synthesis of group 5 transition metal dichalcogenide thin films Kwak, Junghyeok; Jung, Sunshin; Lee, Noho Journal of Materials Chemistry C, Vol. 6, Issue 42 https://doi.org/10.1039/c8tc03909g	journal	January 2018
Unveiling chemical reactivity and oxidation of 1T-phased group VI disulfides Li, Qiang; Shi, Li; Wu, Ruchun Physical Chemistry Chemical Physics, Vol. 21, Issue 31 https://doi.org/10.1039/c9cp02985k	journal	January 2019
P,Se-Codoped MoS ₂ Nanosheets as Accelerated Electrocatalysts for Hydrogen Evolution Zhu, Ting; Ding, Jiabao; Shao, Qi ChemCatChem, Vol. 11, Issue 2 https://doi.org/10.1002/cctc.201801541	journal	December 2018
Analysis of Trends and Emerging Technologies in Water Electrolysis Research Based on a Computational Method: A Comparison with Fuel Cell Research Ogawa, Takaya; Takeuchi, Mizutomo; Kajikawa, Yuya Sustainability, Vol. 10, Issue 2 https://doi.org/10.3390/su10020478	journal	February 2018
High‐Resolution Electrochemical Mapping of the Hydrogen Evolution Reaction on Transition‐Metal Dichalcogenide Nanosheets Takahashi, Yasufumi; Kobayashi, Yu; Wang, Ziqian Angewandte Chemie, Vol. 132, Issue 9 https://doi.org/10.1002/ange.201912863	journal	January 2020
Balancing Light Absorption and Charge Transport in Vertical SnS ₂ Nanoflake Photoanodes with Stepped Layers and Large Intrinsic Mobility Giri, Binod; Masroor, Maryam; Yan, Tao Advanced Energy Materials, Vol. 9, Issue 31 https://doi.org/10.1002/aenm.201901236	journal	July 2019
Nickel@Nitrogen-Doped Carbon@MoS ₂ Nanosheets: An Efficient Electrocatalyst for Hydrogen Evolution Reaction Shah, Sayyar Ali; Shen, Xiaoping; Xie, Minghua Small, Vol. 15, Issue 9 https://doi.org/10.1002/smll.201804545	journal	January 2019
Impact of H-termination on the nitrogen reduction reaction of molybdenum carbide as an electrochemical catalyst Li, Qinye; Qiu, Siyao; He, Lizhong Physical Chemistry Chemical Physics, Vol. 20, Issue 36 https://doi.org/10.1039/c8cp04474k	journal	January 2018
Highly active single-layer MoS ₂ catalysts synthesized by swift heavy ion irradiation Madauß, Lukas; Zegkinoglou, Ioannis; Vázquez Muiños, Henrique Nanoscale, Vol. 10, Issue 48 https://doi.org/10.1039/c8nr04696d	journal	January 2018
Role of oxygen adsorption in modification of optical and surface electronic properties of MoS ₂ Shakya, Jyoti; Kumar, Sanjeev; Mohanty, Tanuja Journal of Applied Physics, Vol. 123, Issue 16 https://doi.org/10.1063/1.5023022	journal	April 2018
Tailoring Active Sites in Mesoporous Defect‐Rich NC/V _o ‐WON Heterostructure Array for Superior Electrocatalytic Hydrogen Evolution Zhang, Bo; Hou, Jungang; Wu, Yunzhen Advanced Energy Materials, Vol. 9, Issue 12 https://doi.org/10.1002/aenm.201803693	journal	January 2019
Synergetic Exfoliation and Lateral Size Engineering of MoS ₂ for Enhanced Photocatalytic Hydrogen Generation Yin, Lisha; Hai, Xiao; Chang, Kun Small, Vol. 14, Issue 14 https://doi.org/10.1002/smll.201704153	journal	March 2018
Structurally Deformed MoS ₂ for Electrochemically Stable, Thermally Resistant, and Highly Efficient Hydrogen Evolution Reaction Chen, Yen-Chang; Lu, Ang-Yu; Lu, Ping Advanced Materials, Vol. 29, Issue 44 https://doi.org/10.1002/adma.201703863	journal	October 2017
Revisiting the Role of Active Sites for Hydrogen Evolution Reaction through Precise Defect Adjusting Zhuang, Peiyuan; Sun, Yangye; Dong, Pei Advanced Functional Materials, Vol. 29, Issue 33 https://doi.org/10.1002/adfm.201901290	journal	June 2019
Activation of MoS ₂ Basal Planes for Hydrogen Evolution by Zinc Wu, Wenzhuo; Niu, Chunyao; Wei, Cong Angewandte Chemie International Edition, Vol. 58, Issue 7 https://doi.org/10.1002/anie.201812475	journal	January 2019
Tungsten nitride/carbide nanocomposite encapsulated in nitrogen-doped carbon shell as an effective and durable catalyst for hydrogen evolution reaction Xu, Shihao; Chu, Suyun; Yang, Liang New Journal of Chemistry, Vol. 42, Issue 24 https://doi.org/10.1039/c8nj04663h	journal	January 2018
Proposal of a stable B ₃ S nanosheet as an efficient hydrogen evolution catalyst Wu, Hong; Li, Xingxing; Zhang, Ruiqi Journal of Materials Chemistry A, Vol. 7, Issue 8 https://doi.org/10.1039/c8ta11797g	journal	January 2019
Recent Development of Metallic (1T) Phase of Molybdenum Disulfide for Energy Conversion and Storage Lei, Zhendong; Zhan, Jing; Tang, Liang Advanced Energy Materials, Vol. 8, Issue 19 https://doi.org/10.1002/aenm.201703482	journal	March 2018
High performance NO ₂ sensor using MoS ₂ nanowires network Kumar, Rahul; Goel, Neeraj; Kumar, Mahesh Applied Physics Letters, Vol. 112, Issue 5 https://doi.org/10.1063/1.5019296	journal	January 2018
Thermal annealing effects on the electrophysical characteristics of sputtered MoS ₂ thin films by Hall effect measurements Qi, Meng; Xiao, Jianrong; Gong, Chenyang Semiconductor Science and Technology, Vol. 34, Issue 4 https://doi.org/10.1088/1361-6641/ab09a5	journal	March 2019
Electrodeposition of amorphous molybdenum sulfide thin film for electrochemical hydrogen evolution reaction Zhang, Lina; Wu, Liangliu; Li, Jing BMC Chemistry, Vol. 13, Issue 1 https://doi.org/10.1186/s13065-019-0600-0	journal	July 2019
A Facile Strategy to Construct Amorphous Spinel-Based Electrocatalysts with Massive Oxygen Vacancies Using Ionic Liquid Dopant Sun, Jing; Guo, Niankun; Shao, Zhiyu Advanced Energy Materials, Vol. 8, Issue 27 https://doi.org/10.1002/aenm.201800980	journal	August 2018
Edge-Terminated MoS ₂ Nanoassembled Electrocatalyst via In Situ Hybridization with 3D Carbon Network Chung, Dong Young; Yoo, Ji Mun; Park, Subin Small, Vol. 14, Issue 36 https://doi.org/10.1002/smll.201802191	journal	August 2018
Multifunctional Carbon-Based Metal-Free Electrocatalysts for Simultaneous Oxygen Reduction, Oxygen Evolution, and Hydrogen Evolution Hu, Chuangang; Dai, Liming Advanced Materials, Vol. 29, Issue 9 https://doi.org/10.1002/adma.201604942	journal	December 2016
Fine Tuning Electronic Structure of Catalysts through Atomic Engineering for Enhanced Hydrogen Evolution Huang, Yichao; Hu, Jun; Xu, Haoxiang Advanced Energy Materials, Vol. 8, Issue 24 https://doi.org/10.1002/aenm.201800789	journal	June 2018
Activation of MoS ₂ Basal Planes for Hydrogen Evolution by Zinc Wu, Wenzhuo; Niu, Chunyao; Wei, Cong Angewandte Chemie, Vol. 131, Issue 7 https://doi.org/10.1002/ange.201812475	journal	January 2019
A mechanism study on the hydrogen evolution reaction catalyzed by molybdenum disulfide complexes Yang, Ti-Long; Ni, Shao-Fei; Qin, Peng Chemical Communications, Vol. 54, Issue 9 https://doi.org/10.1039/c7cc08632f	journal	January 2018
Hybrid catalyst with monoclinic MoTe ₂ and platinum for efficient hydrogen evolution Seok, Jinbong; Lee, Jun-Ho; Bae, Dongyeon APL Materials, Vol. 7, Issue 7 https://doi.org/10.1063/1.5094957	journal	July 2019
MoS₂ Nanosheets Supported on Hollow Carbon Spheres as Efficient Catalysts for Electrochemical Hydrogen Evolution Reaction Li, Wenyue; Zhang, Zhenyu; Zhang, Wenjun ACS Omega, Vol. 2, Issue 8 https://doi.org/10.1021/acsomega.7b00755	journal	August 2017
Catalytic Properties of Vanadium Diselenide: A Comprehensive Study on Its Electrocatalytic Performance in Alkaline, Neutral, and Acidic Media Ulusoy Ghobadi, T. Gamze; Patil, Bhushan; Karadas, Ferdi ACS Omega, Vol. 2, Issue 11 https://doi.org/10.1021/acsomega.7b01226	journal	November 2017

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