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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Electron Irradiation Induces the Conversion from 2H-WSe2 to 1T-WSe2 and Promotes the Performance of Electrocatalytic Hydrogen Evolution

Xiaoqing Yue,Jianqun Yang,Weiqi Li,Yuhang Jing,Lei Dong,Yubao Zhang,Xingji Li

Hydrogen (H2) is an environment-friendly clean energy. In recent years, novel hydrogen evolution electrocatalysts have attracted extensive attention in the scientific community. In this work, the conversion of 2H phase tungsten selenide (2H-WSe2) into 1T phase tungsten selenide (1T-WSe2) was induced by 1 MeV electron irradiation to improve its electrocatalytic performance. When the irradiation fluence is 5 × 1014 e/cm2, the minimum initial overpotential of WSe2 is 101 mV lower than the initial overpotential of WSe2 without irradiation. This method has the characteristics for a simple process and mass production. At the same time, the atomic structure of WSe2 was characterized and the 1T properties of WSe2 were confirmed. The experimental results show that 1 MeV electron irradiates WSe2 to produce Se vacancies on the base surface to form 1T-WSe2, which is the main reason for improving its performance. This effective and feasible electron irradiation method provides a new strategy for the controllable acquisition of 1T-WSe2 and a new method for other similar materials to introduce the ideal 1T phase.

研究领域: 材料科学 · 电催化 · 能源转换
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Activating and optimizing the In-Plane interface of 1 T/2H MoS2 for efficient hydrogen evolution reaction

Kunjie Wang,Yan Jing,Shuang Gao,Xianrong Liu,Bingxin Liu,Yongcheng Li,Peng Zhang,Benhua Xu

Implanting the octahedral phase (1 T) into the hexagonal phase (2H) of the molybdenum disulfide (MoS 2 ) matrix is considered one of the effective methods to enhance hydrogen evolution reaction (HER) performances of MoS 2 . In this paper, hybrid 1 T/2H MoS 2 nanosheets array was successfully grown on conductive carbon cloth (1 T/2H MoS 2 /CC) via facile hydrothermal method and the 1 T phase content in 1 T/2H MoS 2 is regulated to gradually increase from 0 % to 80 %. 1 T/2H MoS 2 /CC with 75 % 1 T phase content exhibits optimal HER performances. The DFT calculation results show that S atoms in 1 T/2H MoS 2 interface exhibit the lowest hydrogen adsorption Gibbs free energies (ΔG H* ) compared with other sites. The improvement of HER performances are primarily attributed to activating the in-plane interface regions of the hybrid 1 T/2H MoS 2 nanosheets. Furthermore, the relationship between 1 T MoS 2 content in 1 T/2H MoS 2 and catalytic activity was simulated by a mathematical model, which shows that the catalytic activity presents a trend of increasing and then decreasing with the increase of 1 T phase content.

研究领域: 材料科学 · 理论计算 · 电催化
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

One-Step Synthesis of Porous FeNiSx Coupled with 1T/2H MoS2 via Hydrazine Hydrate-Induced Phase Transformation for Hydrogen Evolution

Huangcong Tang,Jiayang Dou,Zhixian He,Jingwen An,Wenhuan Liu,Sheying Dong

Heterostructured catalysts with the potential synergies between the polymetallic sulfides and the construction of 1T-phase MoS2 are a promising alternative and contribute to obtain the enhanced hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance. Herein, the porous hybrid nanostructures coupling FeS2 and NiS complexes with 1T/2H phase MoS2 (FeNiSx@MoS2–HZHx) are prepared via a facile one-pot pyrolysis strategy accompanied by hydrazine hydrate (HZH)-induced phase transformation without the assistance of a template. The hybrid nanostructures possessing crystalline–amorphous (c–a) interface need overpotentials of 139 mV to achieve the current density of 10 mA cm–2 (η10) in 0.5 M H2SO4, which have superior kinetics for the HER process with a Tafel slope value of 57.9 mV dec–1. The 24 h continuous HER operated at η10 exhibits negligible deterioration, which has only a decrease of 3 mV at η10 after the 5000 cyclic voltammetry cycle tests, indicating the desirable stability of FeNiSx@MoS2–HZH2. Beyond that, the resultant FeNiSx@MoS2 requires 335 mV at η10. Specifically, the electrochemical and structural characterization prove that the enhanced HER performance is contributed from the incorporation of HZH to form FeS2/MoS2/NiS heterostructures and c–a interface sites coupling with 1T/2H phase MoS2, which provide more exposed active sites benefiting from the larger surface area. The simple and convenient design strategy has certain enlightenment for the development of sustainable energy production.

研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Mixed 1T-2H phase MoSe2 as interfacial charge-transfer-bridge to boosting photocatalytic activity of dual Z-scheme AgI/1T-2H MoSe2/Bi4O5Br2 heterojunction

Yi Wang,Xinyan Xiao,Tingting Ding,Mingli Lu

The transition-metal dichalcogenides (TMDs) with 1T phase structure holds great promise for providing abundant active sites and superior conductivity, while the achievement of highly efficient degradation activity over bare TMDs and TMDs-based photocatalysts is still challenges. In this work, a flower-like mixed 1T-2H phase MoSe 2 was synthesized via a sodium borohydride (NaBH 4 )-assisted solvothermal method, and then was selected as a “charge-transfer-bridge” to fabricate a dual Z-scheme AgI/1T-2H MoSe 2 /Bi 4 O 5 Br 2 composite with a 0D/3D hierarchical structure. The optimal AgI/1T-2H MoSe 2 /Bi 4 O 5 Br 2 composite exhibited the superior photocatalytic activity towards degrading RhB and TC relative to AgI/2H MoSe 2 /Bi 4 O 5 Br 2 and AgI/Bi 4 O 5 Br 2 . The enhancement is attributed to its better light absorption, abundant active sites, and superior charge carrier mobility and separation efficiency, resulted from synergetic effect of 0D/3D structural coupling and energy band matching. Moreover, the important energy band alignments and mixed 1T-2H phase MoSe 2 boosting photocatalytic mechanism of as-prepared AgI/1T-2H MoSe 2 /Bi 4 O 5 Br 2 heterojunction were investigated. This work describes a competitive design and fabrication technique for constructing novel mixed phase TMDs-based Z-scheme heterojunctions to address environmental issues.

研究领域: 材料科学 · 环境科学
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FUEL · 2022 · IF 8.035

Symbiosis of 1 T and 2H phases in the basal plane of defective MoS2 nanoflowers for efficient hydrodesulfurization

Zhe Bai,Luyao Wang,Hongwei Cao,Xiangwen Zhang,Guozhu Li

Hydrodesulfurization (HDS) is an effective way to reduce sulfur content in oil for the enforcement of more stringent environmental regulations. MoS 2 has been widely used as an effective component for catalyzing HDS, and needs to be extensively studied in depth. Herein, MoS 2 nanoflowers with the symbiosis of 1T-2H phases in the basal planes and coexistence of S and Mo vacancies are prepared via the assembly of many nanosheets by a one-pot solvothermal method. The morphology, crystal phase structure and defects of these 1T-2H MoS 2 samples were well characterized. The 1T/2H ratio and the state of vacancies were effectively tuned by changing the solvothermal conditions. Active and stable 1T-2H mixed MoS 2 nanoflowers with high content of 1T phase and moderate S and Mo vacancies were obtained by the regulation of oxalic acid in the mixture of ethanol and water. In the HDS of dibenzothiophene at 300 °C and 4 MPa, the optimal catalyst of MoS 2 -water–ethanol-OA exhibited a substrate conversion of 89.3% in 10 h. Moreover, the activity of MoS 2 -water–ethanol-OA was well retained without any decrease in the recycling experiment.

CAS / MDL: 12054-85-2
研究领域: 催化 · 材料科学 · 化学工程
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RARE METALS · 2023 ·Vol. 42 ·期 12 ·3985-3992 · IF 8.8

Chemical vapor deposition synthesis of V-doped MoS2

Yang Yang,Liang Qing-Rong,Zhu Chun-Li,Zheng Guo-Zhong,Zhang Jian,Zheng Shou-Jun,Lin Yung-Chang,Zheng De-Zhi,Zhou Jia-Dong

Van der Waals coupling with different stacking configurations can significantly affect the optical and electronic properties of ultrathin two-dimensional (2D) materials, which is an effective way to tune device performance. Herein, we report a salt-assisted chemical vapor deposition method for the synthesis of bilayer V-doped MoS 2 with 2H and 3R phases, which are demonstrated by the second harmonic generation and scanning transmission electron microscopy. Notably, the mobility of the 3R phase V-doped MoS 2 is 6.2% higher than that of the 2H phase. Through first-principles calculations, we further reveal that this particular behavior is attributed to the stronger interlayer coupling of 3R compared to the 2H stacking configuration. This research can be further generalized to other transition metal chalcogenides and will contribute to the development of electronic devices based on 2D materials in the future.

研究领域: 材料科学 · 纳米科技 · 凝聚态物理 · 二维材料 · 半导体材料 · 表面科学 · 计算材料学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2020 · IF 6.155

Freestanding nanosheets of 1T-2H hybrid MoS2 as electrodes for efficient sodium storage

Haiyang Yu,Zhenzhu Wang,Jiangfeng Ni,Liang Li

Molybdenum disulfide (MoS 2 ) is a promising electrode material for sodium-ion batteries as it offers a large capacity through a distinct conversion reaction. However, the electrochemical potential of MoS 2 is often restrained by the poor conductivity as the dominant 2H phase is a semiconductor while the metallic 1T phase is thermodynamically unstable. In this work, we report a hybrid design and material preparation of freestanding nanosheets of MoS 2 composed of both 1T and 2H phases based on mild hydrothermal reaction . The introduction of the metallic 1T-MoS 2 phase into 2H-MoS 2 and their intimate hybridization enable a significant improvement in electronic conductivity, while the freestanding architecture avoids possible electrochemical aggregation. When used as electrodes for sodium storage, such a hybrid MoS 2 affords a high capacity of ∼500 mA h g −1 at 0.5 A g −1 after 300 cycles, and retains capacity of ∼200 mA h g −1 at a high current rate of 4 A g −1 , thus demonstrating their potential in high-performance battery applications.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 无机化学
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Nature Synthesis · 2024 · IF 0

Phase-switchable preparation of solution-processable WS2 mono- or bilayers

Mei Liang,Gao Zhan,Yang Ruijie,Zhang Zhen,Sun Mingzi,Liang Xiongyi,Zhang Yuefeng,Ying Ting,Hu Honglu,Li Dengfeng,Zhang Qinghua,Gu M. Danny,Gu Lin,Zhou Jiang,Huang Bolong,Voiry Damien,Zeng Xiao Cheng,Chai Yang,Li Ju,Yu Xinge,Zeng Zhiyuan

Crystal phase plays a crucial role in determining the properties of two-dimensional (2D) transition metal dichalcogenides. Here we achieve phase-switchable preparation of 2D transition metal dichalcogenides using an electrochemical lithium-ion intercalation-based exfoliation strategy by controlling the discharge current density and cutoff voltage. We discover that a small discharge current density (0.005 A g −1 , with a 0.9 V cutoff voltage) produces pure semiconducting 2H phase WS 2 bilayers. In contrast, a large discharge current density (0.02 A g −1 , with a 0.7 V cutoff voltage) leads to the dominant semimetallic 1T′ phase WS 2 monolayers. The phase-switching mechanism was clarified through cryo-electron microscopy, annular dark-field scanning transmission electron microscopy, Raman, X-ray photoelectron spectroscopy, etc. The device (humidity sensor) application of produced 2D WS 2 was then demonstrated, showing phase-dependent humidity-sensing performances confirming the potential of our produced 2D WS 2 with switchable phase in device applications.

CAS / MDL: 919-30-2
研究领域: 材料科学 · 纳米技术 · 电化学 · 传感器
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LANGMUIR · 2025 · IF 3.9

1T/2H-MoS2 Nanoclusters as Plasmon-Free Surface-Enhanced Raman Spectroscopy Substrates for Ultrasensitive Detection of Environmental Pollutants

Zhenyu Wen,Wenjie Zhu,Yongxue Chen,Huanhuan Sun,Lin Zhu,Yuling Yang,Yanping Song,Lei Chen,Jiajun Dong,Bingbing Liu

Surface-enhanced Raman spectroscopy (SERS) holds immense promise for molecular detection, yet the quest for high-performance, plasmon-free substrates remains active. This work pioneers the rational design and engineering of phase-tunable MoS2 nanoclusters─metallic (1T), semiconductor (2H), and, critically, hybrid metal/semiconductor (1T/2H) phases as a novel class of SERS platforms. We demonstrate this exceptional capability for ultrasensitive detection of environmentally hazardous dyes (e.g., rhodamine B, crystal violet, and methylene blue). Remarkably, the optimized 1T/2H-MoS2 substrate achieves an enhancement factor of 1.02 × 109, which ranks among the higher values for SERS substrates derived from semiconductors. Crucially, time-resolved transient photoluminescence decay spectroscopy reveals a dramatic 52% decrease in average exciton lifetime (from 3.88 to 1.86 ns) for RhB adsorbed on 1T/2H-MoS2 substrates. This profound decrease provides direct evidence for highly efficient interfacial charge transfer, predominantly driven by the built-in electric field unique to the engineered phase junction. Furthermore, by leveraging the distinct Raman signatures enabled by this heterophase substrate, we achieve the multiplex detection of all five environmental nucleobases (adenine, guanine, cytosine, thymine, and uracil) in both individual and mixed solutions. This work not only delivers fundamental mechanistic insights into charge transfer-mediated SERS but also provides a practical platform with broad implications for environmental monitoring, biomedical diagnostics, and analytical chemistry.

研究领域: 分析化学 · 环境科学 · 纳米技术 · 光谱学 · 材料科学 · 生物医学诊断
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Carbon Energy · 2022 ·Vol. 5 ·期 2 ·e255 · IF 21.556

Li intercalation in an MoSe2 electrocatalyst: In situ observation and modulation of its precisely controllable phase engineering for a high-performance flexible Li-S battery

Yunke Wang,Yige Zhao,Kangli Liu,Shaobin Wang,Neng Li,Guosheng Shao,Feng Wang,Peng Zhang

Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries (LSBs). Phase transformation of MoSe 2 from the 2H phase to the 1T phase has been proven to be a significant method to improve the catalytic activity. However, precisely controllable phase engineering of MoSe 2 has rarely been reported. Herein, by in situ Li ions intercalation in MoSe 2 , a precisely controllable phase evolution from 2H-MoSe 2 to 1T-MoSe 2 was realized. More importantly, the definite functional relationship between cut-off voltage and phase structure was first identified for phase engineering through in situ observation and modulation methods. The sulfur host (CNFs/1T-MoSe 2 ) presents high charge density, strong polysulfides adsorption, and catalytic kinetics. Moreover, Li-S cells based on it display capacity retention of 875.3 mAh g −1 after 500 cycles at 1 C and an areal capacity of 8.71 mAh cm −2 even at a high sulfur loading of 8.47 mg cm −2 . Furthermore, the flexible pouch cell exhibiting decent performance will endow a promising potential in the wearable energy storage field. This study proposes an effective strategy to precisely control the phase structure of MoSe 2 , which may provide the reference to fabricate the highly efficient electrocatalysts for LSBs and other energy systems.

研究领域: 材料科学 · 电化学 · 储能技术 · 纳米技术 · 电池技术
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