Critical review: hydrothermal synthesis of 1T-MoS2 – an important route to a promising material

The unique anisotropy, polytypism, and abundance of molybdenum disulfide make it a singularly versatile material for a range of catalytic, electrochemical, and tribological applications. By employing a hydrothermal synthesis, a high surface area, optionally-supported, gas-repellent metallic MoS2 (1T-MoS2) has been reported to be produced from benign reagents at scale. This hydrothermally produced material has been shown to exhibit outstanding performance as a capacitor, and as an electrocatalyst (e.g. for the hydrogen evolution reaction). However, synthetic ambiguity and sample mischaracterizations are extremely common within the literature of reports of hydrothermally produced 1T-MoS2, and these occur across a range of analysis techniques such as Raman spectroscopy, X-ray diffraction, magnetic susceptibility, and X-ray photoelectron spectroscopy. These oversights have led to significant inconsistencies in the prevalent understanding of 1T-MoS2. In most cases in the literature it is unclear whether MoS2 or an intercalated (Mn+)(1/n)MoIIIS2− variant is produced. Given the high potential of this material for many cutting-edge applications, it is important to clarify the literature to help facilitate rapid progress. In this context the review presents a way forward, by setting out to provide clear and unambiguous synthetic and analytical strategies.

[1]  Jeunghee Park,et al.  Two-dimensional MoS2–melamine hybrid nanostructures for enhanced catalytic hydrogen evolution reaction , 2019, Journal of Materials Chemistry A.

[2]  S. Miao,et al.  Vertical nanosheet array of 1T phase MoS2 for efficient and stable hydrogen evolution , 2019, Applied Catalysis B: Environmental.

[3]  Fangming Jin,et al.  Phase-selective Hydrothermal Synthesis of Metallic MoS2 at High Temperature , 2019, Chemistry Letters.

[4]  Yan‐Zhen Zheng,et al.  One-step hydrothermal synthesis of high-percentage 1T-phase MoS2 quantum dots for remarkably enhanced visible-light-driven photocatalytic H2 evolution , 2019, Applied Catalysis B: Environmental.

[5]  Minbaek Lee,et al.  Facile microwave assisted synthesis of vastly edge exposed 1T/2H-MoS2 with enhanced activity for hydrogen evolution catalysis , 2019 .

[6]  S. Dou,et al.  Highly Ambient-Stable 1T-MoS2 and 1T-WS2 by Hydrothermal Synthesis under High Magnetic Fields. , 2019, ACS nano.

[7]  Y. Hu,et al.  Synthesis, stabilization and applications of 2-dimensional 1T metallic MoS2 , 2018 .

[8]  Wei Zhao,et al.  Metastable MoS2 : Crystal Structure, Electronic Band Structure, Synthetic Approach and Intriguing Physical Properties. , 2018, Chemistry.

[9]  S. Pennycook,et al.  Differentiating Polymorphs in Molybdenum Disulfide via Electron Microscopy , 2018, Advanced materials.

[10]  C. Xiong,et al.  In situ growth of 1T-MoS2 on liquid-exfoliated graphene: A unique graphene-like heterostructure for superior lithium storage , 2018, Carbon.

[11]  Jeunghee Park,et al.  Intercalation of aromatic amine for the 2H-1T' phase transition of MoS2 by experiments and calculations. , 2018, Nanoscale.

[12]  C. Karthik,et al.  Paramagnetic defects in hydrothermally grown few-layered MoS_2 nanocrystals , 2018, Journal of Materials Research.

[13]  Jeunghee Park,et al.  Stable methylammonium-intercalated 1T′-MoS2 for efficient electrocatalytic hydrogen evolution , 2018 .

[14]  Hua Zhang,et al.  High phase-purity 1T′-MoS2- and 1T′-MoSe2-layered crystals , 2018, Nature Chemistry.

[15]  A. Dalton,et al.  Considerations for spectroscopy of liquid-exfoliated 2D materials: emerging photoluminescence of N-methyl-2-pyrrolidone , 2017, Scientific Reports.

[16]  Wenjun Zhang,et al.  Interlayer Nanoarchitectonics of Two‐Dimensional Transition‐Metal Dichalcogenides Nanosheets for Energy Storage and Conversion Applications , 2017 .

[17]  M. Rajamathi,et al.  Magnetic Co-Doped MoS2 Nanosheets for Efficient Catalysis of Nitroarene Reduction , 2017, ACS omega.

[18]  Lijun Wang,et al.  Metallic 1T MoS2 nanosheet arrays vertically grown on activated carbon fiber cloth for enhanced Li-ion storage performance , 2017 .

[19]  R. Hurt,et al.  Oxidation suppression during hydrothermal phase reversion allows synthesis of monolayer semiconducting MoS2 in stable aqueous suspension. , 2017, Nanoscale.

[20]  Yanzhi Xia,et al.  Synthetic methods and potential applications of transition metal dichalcogenide/graphene nanocomposites , 2016 .

[21]  A. Hanbicki,et al.  Dynamics of chemical vapor sensing with MoS2 using 1T/2H phase contacts/channel. , 2016, Nanoscale.

[22]  W. Que,et al.  Molybdenum disulfide nanomaterials: Structures, properties, synthesis and recent progress on hydrogen evolution reaction , 2016 .

[23]  Hongli Zhu,et al.  Pure and stable metallic phase molybdenum disulfide nanosheets for hydrogen evolution reaction , 2016, Nature Communications.

[24]  Xiuling Li,et al.  Gram-Scale Aqueous Synthesis of Stable Few-Layered 1T-MoS2 : Applications for Visible-Light-Driven Photocatalytic Hydrogen Evolution. , 2015, Small.

[25]  M. Pumera,et al.  Electrochemistry of Nanostructured Layered Transition-Metal Dichalcogenides. , 2015, Chemical reviews.

[26]  T. Heinz,et al.  Probing the Dynamics of the Metallic-to-Semiconducting Structural Phase Transformation in MoS2 Crystals. , 2015, Nano letters.

[27]  M. Chhowalla,et al.  Metallic 1T phase MoS2 nanosheets as supercapacitor electrode materials. , 2015, Nature nanotechnology.

[28]  A. Mohite,et al.  Phase engineering of transition metal dichalcogenides. , 2015, Chemical Society reviews.

[29]  Yunhui Huang,et al.  Nanostructured Mo-based electrode materials for electrochemical energy storage. , 2015, Chemical Society reviews.

[30]  Charles C. L. McCrory,et al.  Benchmarking hydrogen evolving reaction and oxygen evolving reaction electrocatalysts for solar water splitting devices. , 2015, Journal of the American Chemical Society.

[31]  Cory M. Simon,et al.  Correction: Corrigendum: Kinetically tuned dimensional augmentation as a versatile synthetic route towards robust metal–organic frameworks , 2015, Nature Communications.

[32]  Youwei Du,et al.  Enhancement of magnetism by structural phase transition in MoS2 , 2015 .

[33]  Hua Zhang,et al.  The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. , 2013, Nature chemistry.

[34]  Hisato Yamaguchi,et al.  Photoluminescence from chemically exfoliated MoS2. , 2011, Nano letters.

[35]  R. Tenne,et al.  New Route for Stabilization of 1T-WS2 and MoS2 Phases , 2011, 1110.3848.

[36]  N. Tsuchiya,et al.  Sustainable hydrogen production system with sulfur–water–organic materials by hydrothermal reaction , 2008 .

[37]  A. Sahibed-dine,et al.  Evidence of the reverse Claus reaction on metal oxides: Influence of their acid–base properties , 2000 .

[38]  C. Lenardi,et al.  XPS investigation of preferential sputtering of S from MoS2 and determination of MoSx stoichiometry from Mo and S peak positions , 1999 .

[39]  A. Dent,et al.  In Situ Investigation of the Thermal Decomposition of Ammonium Tetrathiomolybdate Using Combined Time-Resolved X-ray Absorption Spectroscopy and X-ray Diffraction , 1998 .

[40]  L. Thompson,et al.  XPS study of as-prepared and reduced molybdenum oxides , 1996 .

[41]  J. Lassègues,et al.  Infrared and Raman spectra of MoO 3 molybdenum trioxides and MoO 3 · xH 2O molybdenum trioxide hydrates , 1995 .

[42]  F. Lévy,et al.  Random stacking in MoS2−x sputtered thin films , 1994 .

[43]  Yang,et al.  Raman study and lattice dynamics of single molecular layers of MoS2. , 1991, Physical review. B, Condensed matter.

[44]  G. George,et al.  L-edge spectroscopy of molybdenum compounds and enzymes , 1990 .

[45]  P. Mulhern Lithium intercalation in crystalline LixMoS2 , 1989 .

[46]  A. Guinier,et al.  Nomenclature of Polytype Structures Report of the International Union of Crystallography Ad-Hoc Committee on the Nomenclature of Disordered, Modulated and Polytype Structures* , 1984 .

[47]  E. Prestridge,et al.  Molybdenum Disulfide in the Poorly Crystalline "Rag" Structure , 1979, Science.

[48]  L. Mattheiss Band Structures of Transition-Metal-Dichalcogenide Layer Compounds. , 1973 .

[49]  A. Müller,et al.  Thermal decomposition of (NH4)2MoO2S2, (NH4)2MoS4, (NH4)2WO2S2 and (NH4)2WS4 , 1973 .

[50]  R. Somoano,et al.  Alkali metal intercalates of molybdenum disulfide. , 1973 .

[51]  W. Rüdorff,et al.  Einlagerungsverbindungen von Alkali- und Erdalkalimetallen in Molybdän- und Wolframdisulfid , 1959 .

[52]  P. Aneesh,et al.  Phase Engineering from 2H to 1T-MoS2 for Efficient Ammonia PL Sensor and Electrocatalyst for Hydrogen Evolution Reaction , 2019, Journal of The Electrochemical Society.

[53]  G. Thompson,et al.  Synthesis and characterization of molybdenum disulphide formed from ammonium tetrathiomolybdate , 1997 .

[54]  F. Wypych,et al.  1T-MoS2, a new metallic modification of molybdenum disulfide , 1992 .

[55]  A. Masters,et al.  Applications of molybdenum-95 N.M.R. spectroscopy. X. Polyoxomolybdates , 1984 .

[56]  R. R. Haering,et al.  Structural destabilization induced by lithium intercalation in MoS2 and related compounds , 1983 .