Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction

Cummins, Dustin R.; Martinez, Ulises; Sherehiy, Andriy; Kappera, Rajesh; Martinez-Garcia, Alejandro; Schulze, Roland K.; Jasinski, Jacek; Zhang, Jing; Gupta, Ram K.; Lou, Jun; Chhowalla, Manish; Sumanasekera, Gamini; Mohite, Aditya D.; Sunkara, Mahendra K.; Gupta, Gautam

doi:10.1038/ncomms11857

Title: Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction

Journal Article · Fri Jun 10 00:00:00 EDT 2016 · Nature Communications

DOI: https://doi.org/10.1038/ncomms11857 · OSTI ID:1341863

^[1]; Martinez, Ulises ^[2]; Sherehiy, Andriy ^[3]; Kappera, Rajesh ^[4]; Martinez-Garcia, Alejandro ^[3]; Schulze, Roland K. ^[2]; Jasinski, Jacek ^[3]; Zhang, Jing ^[5]; Gupta, Ram K. ^[6]; Lou, Jun ^[5]; Chhowalla, Manish ^[7]; Sumanasekera, Gamini ^[3]; Mohite, Aditya D. ^[2]; Sunkara, Mahendra K. ^[3]; Gupta, Gautam ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Louisville, Louisville, KY (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Louisville, Louisville, KY (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rutgers Univ., Piscataway, NJ (United States)
Rice Univ., Houston, TX (United States)
Pittsburg State Univ., Pittsburg, KS (United States)
Rutgers Univ., Piscataway, NJ (United States)

In this study, hydrogen evolution reaction is catalyzed efficiently with precious metals, such as platinum; however, transition metal dichalcogenides have recently emerged as a promising class of materials for electrocatalysis, but these materials still have low activity and durability when compared with precious metals. Here we report a simple one-step scalable approach, where MoO_x/MoS₂ core-shell nanowires and molybdenum disulfide sheets are exposed to dilute aqueous hydrazine at room temperature, which results in marked improvement in electrocatalytic performance. The nanowires exhibit ~100 mV improvement in over potential following exposure to dilute hydrazine, while also showing a 10-fold increase in current density and a significant change in Tafel slope. In situ electrical, gate-dependent measurements and spectroscopic investigations reveal that hydrazine acts as an electron dopant in molybdenum disulfide, increasing its conductivity, while also reducing the MoO_x core in the core-shell nanowires, which leads to improved electrocatalytic performance.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1341863

Report Number(s):: LA-UR--16-23488

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Kinetic‐Oriented Construction of MoS ₂ Synergistic Interface to Boost pH‐Universal Hydrogen Evolution Hu, Jue; Zhang, Chengxu; Yang, Peng Advanced Functional Materials, Vol. 30, Issue 6 https://doi.org/10.1002/adfm.201908520	journal	December 2019
Ternary Porous Cobalt Phosphoselenide Nanosheets: An Efficient Electrocatalyst for Electrocatalytic and Photoelectrochemical Water Splitting Hou, Yang; Qiu, Ming; Zhang, Tao Advanced Materials, Vol. 29, Issue 35 https://doi.org/10.1002/adma.201701589	journal	July 2017
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
Efficient Hydrogen Production on a 3D Flexible Heterojunction Material Yu, Huidi; Xue, Yurui; Hui, Lan Advanced Materials, Vol. 30, Issue 21 https://doi.org/10.1002/adma.201707082	journal	April 2018
Metallic Twin Boundaries Boost the Hydrogen Evolution Reaction on the Basal Plane of Molybdenum Selenotellurides Kosmala, Tomasz; Coy Diaz, Horacio; Komsa, Hannu-Pekka Advanced Energy Materials, Vol. 8, Issue 20 https://doi.org/10.1002/aenm.201800031	journal	April 2018
Energy-Saving Electrolytic Hydrogen Generation: Ni ₂ P Nanoarray as a High-Performance Non-Noble-Metal Electrocatalyst Tang, Chun; Zhang, Rong; Lu, Wenbo Angewandte Chemie, Vol. 129, Issue 3 https://doi.org/10.1002/ange.201608899	journal	December 2016
Boron‐Induced Electronic‐Structure Reformation of CoP Nanoparticles Drives Enhanced pH‐Universal Hydrogen Evolution Cao, Erping; Chen, Zhimin; Wu, Hao Angewandte Chemie, Vol. 132, Issue 10 https://doi.org/10.1002/ange.201915254	journal	January 2020
Energy-Saving Electrolytic Hydrogen Generation: Ni ₂ P Nanoarray as a High-Performance Non-Noble-Metal Electrocatalyst Tang, Chun; Zhang, Rong; Lu, Wenbo Angewandte Chemie International Edition, Vol. 56, Issue 3 https://doi.org/10.1002/anie.201608899	journal	December 2016
Boron‐Induced Electronic‐Structure Reformation of CoP Nanoparticles Drives Enhanced pH‐Universal Hydrogen Evolution Cao, Erping; Chen, Zhimin; Wu, Hao Angewandte Chemie International Edition, Vol. 59, Issue 10 https://doi.org/10.1002/anie.201915254	journal	January 2020
Activating the MoS ₂ Basal Plane by Controllable Fabrication of Pores for an Enhanced Hydrogen Evolution Reaction Geng, Shuo; Liu, Hu; Yang, Weiwei Chemistry - A European Journal, Vol. 24, Issue 71 https://doi.org/10.1002/chem.201804658	journal	November 2018
Highly Efficient and Durable Electrocatalyst Based on Nanowires of Cobalt Sulfide for Overall Water Splitting Zhang, Chunyang; Bhoyate, Sanket; Kahol, Pawan K. ChemNanoMat, Vol. 4, Issue 12 https://doi.org/10.1002/cnma.201800301	journal	September 2018
Oxygen Doping to Optimize Atomic Hydrogen Binding Energy on NiCoP for Highly Efficient Hydrogen Evolution Liu, Chunlei; Zhang, Gong; Yu, Li Small, Vol. 14, Issue 22 https://doi.org/10.1002/smll.201800421	journal	April 2018
Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS ₂ /WTe ₂ Hybrid Structures Zhou, Yu; Pondick, Joshua V.; Silva, Jose Luis Small, Vol. 15, Issue 19 https://doi.org/10.1002/smll.201900078	journal	April 2019
Hydrogen adsorption engineering by intramolecular proton transfer on 2D nanosheets Lee, Hanleem; Bak, Sora; Cho, Yunhee NPG Asia Materials, Vol. 10, Issue 5 https://doi.org/10.1038/s41427-018-0037-2	journal	May 2018
Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis Wu, Yishang; Liu, Xiaojing; Han, Dongdong Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03858-w	journal	April 2018
Engineering stepped edge surface structures of MoS ₂ sheet stacks to accelerate the hydrogen evolution reaction Hu, Jue; Huang, Bolong; Zhang, Chengxu Energy & Environmental Science, Vol. 10, Issue 2 https://doi.org/10.1039/c6ee03629e	journal	January 2017
A reduced graphene oxide/mixed-valence manganese oxide composite electrode for tailorable and surface mountable supercapacitors with high capacitance and super-long life Wang, Yang; Lai, Wenhui; Wang, Ni Energy & Environmental Science, Vol. 10, Issue 4 https://doi.org/10.1039/c6ee03773a	journal	January 2017
Direct deposition of MoSe ₂ nanocrystals onto conducting substrates: towards ultra-efficient electrocatalysts for hydrogen evolution Damien, Dijo; Anil, Athira; Chatterjee, Dipanwita Journal of Materials Chemistry A, Vol. 5, Issue 26 https://doi.org/10.1039/c6ta09645j	journal	January 2017
Molybdenum disulfide and Au ultrasmall nanohybrids as highly active electrocatalysts for hydrogen evolution reaction Zhang, Jinxuan; Wang, Tanyuan; Liu, Lu Journal of Materials Chemistry A, Vol. 5, Issue 8 https://doi.org/10.1039/c6ta10385e	journal	January 2017
Highly dispersed palladium nanoparticles generated in situ on layered double hydroxide nanowalls for ultrasensitive electrochemical detection of hydrazine Xu, Liang; Qu, Zongkai; Chen, Jun Analytical Methods, Vol. 9, Issue 47 https://doi.org/10.1039/c7ay02324c	journal	January 2017
Ni–Mo–O nanorod-derived composite catalysts for efficient alkaline water-to-hydrogen conversion via urea electrolysis Yu, Zi-You; Lang, Chao-Chao; Gao, Min-Rui Energy & Environmental Science, Vol. 11, Issue 7 https://doi.org/10.1039/c8ee00521d	journal	January 2018
The atomic origin of nickel-doping-induced catalytic enhancement in MoS ₂ for electrochemical hydrogen production Luo, Ruichun; Luo, Min; Wang, Ziqian Nanoscale, Vol. 11, Issue 15 https://doi.org/10.1039/c8nr10023c	journal	January 2019
An overview on Pd-based electrocatalysts for the hydrogen evolution reaction Sarkar, Shreya; Peter, Sebastian C. Inorganic Chemistry Frontiers, Vol. 5, Issue 9 https://doi.org/10.1039/c8qi00042e	journal	January 2018
A bimetallic oxide Fe _1.89 Mo _4.11 O ₇ electrocatalyst with highly efficient hydrogen evolution reaction activity in alkaline and acidic media Hao, Zhaomin; Yang, Shishuai; Niu, Jingyang Chemical Science, Vol. 9, Issue 25 https://doi.org/10.1039/c8sc01710g	journal	January 2018
Engineering sub-100 nm Mo _(1−x) W _x Se ₂ crystals for efficient hydrogen evolution catalysis Zhuang, Minghao; Gan, Li-Yong; Zou, Mingchu Journal of Materials Chemistry A, Vol. 6, Issue 7 https://doi.org/10.1039/c8ta00082d	journal	January 2018
A platinum oxide decorated amorphous cobalt oxide hydroxide nanosheet array towards alkaline hydrogen evolution Wang, Ziqiang; Ren, Xiang; Shi, Xifeng Journal of Materials Chemistry A, Vol. 6, Issue 9 https://doi.org/10.1039/c8ta00241j	journal	January 2018
Highly active and stable electrocatalyst of Ni ₂ P nanoparticles supported on 3D ordered macro-/mesoporous Co–N-doped carbon for acidic hydrogen evolution reaction Sun, Tingting; Dong, Jing; Huang, Yan Journal of Materials Chemistry A, Vol. 6, Issue 26 https://doi.org/10.1039/c8ta03672a	journal	January 2018
Well dispersed MoC quantum dots in ultrathin carbon films as efficient co-catalysts for photocatalytic H ₂ evolution Gao, Fan; Zhao, Yan; Zhang, Lulu Journal of Materials Chemistry A, Vol. 6, Issue 39 https://doi.org/10.1039/c8ta06029k	journal	January 2018
The controlled construction of a ternary hybrid of monodisperse Ni ₃ S ₄ nanorods/graphitic C ₃ N ₄ nanosheets/nitrogen-doped graphene in van der Waals heterojunctions as a highly efficient electrocatalyst for overall water splitting and a promising anode material for sodium-ion batteries Yang, Jing; Xing, Shiqi; Zhou, Jianbin Journal of Materials Chemistry A, Vol. 7, Issue 8 https://doi.org/10.1039/c8ta07253a	journal	January 2019
Tungsten-inert gas welding electrodes as low-cost, green and pH-universal electrocatalysts for the hydrogen evolution reaction Hashemniaye-Torshizi, Reihaneh; Ashraf, Narges; Arbab-Zavar, Mohammad Hossein New Journal of Chemistry, Vol. 43, Issue 29 https://doi.org/10.1039/c9nj02298h	journal	January 2019
The development of 2D materials for electrochemical energy applications: A mechanistic approach Hynek, David J.; Pondick, Joshua V.; Cha, Judy J. APL Materials, Vol. 7, Issue 3 https://doi.org/10.1063/1.5085187	journal	March 2019
Large-area MoS ₂ -MoO _x heterojunction thin-film photodetectors with wide spectral range and enhanced photoresponse Im, Healin; Liu, Na; Bala, Arindam APL Materials, Vol. 7, Issue 6 https://doi.org/10.1063/1.5094586	journal	June 2019
Surface states in bulk single crystal of topological semimetal Co ₃ Sn ₂ S ₂ toward water oxidation Li, Guowei; Xu, Qiunan; Shi, Wujun Science Advances, Vol. 5, Issue 8 https://doi.org/10.1126/sciadv.aaw9867	journal	August 2019
Modulating the Volmer Step by MOF Derivatives Assembled with Heterogeneous Ni ₂ P-CoP Nanocrystals in Alkaline Hydrogen Evolution Reaction Liang, Da; Jiang, Hao; Xu, Qiucheng Journal of The Electrochemical Society, Vol. 165, Issue 16 https://doi.org/10.1149/2.0131816jes	journal	January 2018
A Renewable Platform for High-Performance Glucose Sensor Based on Co(OH) ₂ Nanoparticles/Three-Dimensional Graphene Frameworks Du, Yongling; He, Yifeng; Zheng, Zhixiang Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.0481902jes	journal	January 2019
MoS2 Decorated Carbon Nanofibers as Efficient and Durable Electrocatalyst for Hydrogen Evolution Reaction Zhang, C.; Wang, Z.; Bhoyate, S. C, Vol. 3, Issue 4 https://doi.org/10.3390/c3040033	journal	October 2017
Surface states in bulk single crystal of topological semimetal Co$_3$Sn$_2$S$_2$ towards water oxidation Li, Guowei; Xu, Qiunan; Shi, Wujun arXiv https://doi.org/10.48550/arxiv.1908.08567	text	January 2019

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