Science China-Materials
·
2021
·Vol. 64
·期 9
·2202-2211
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IF 8.273
Wang Yaqian,Shen Yongli,Xiao Xiong,Dai Linxiu,Yao Shuang,An Changhua
Metastable 1T′ MoTe 2 has attracted much attention as a cost-effective electrocatalyst for hydrogen evolution reaction (HER) in recent years. However, few studies were done over common stable 2H phase because it often exhibits inferior performance. Herein, stable 2H MoTe 2 with S-doped Te vacancies has been synthesized by one-step telluride conversion of 1T MoS 2 at 700°C under Ar/H 2 atmosphere. It is demonstrated that the synergistic effect of S-doping and Te vacancies changes the electronic structures of the catalyst. Density functional theory (DFT) studies show that plentiful electrons accumulate on the surface S atoms in S-doped Te vacancies of 2H MoTe 2 catalyst, which may be as active sites to promote HER. Moreover, the as-synthesized catalyst can be directly used as working electrode, and realizes current density of 100 mA cm −2 at overpotential of 217 mV with Tafel slope of 94 mV dec −1 . This work stimulates intensive studies on the activation of inert phase of other nanocatalysts towards various reactions.
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高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Shuang Gao,Shaoqing Chen,Feng Shi,Wenwen Jiang,Jiafu Chen
Molybdenum disulfide (MoS 2 ), as a classical layered transition-metal dichalcogenide (TMD), shows great potential as an advanced Zn 2+ storage cathode of aqueous Zn-ion batteries (ZIBs) due to high theoretical capacity and two-dimensional Zn 2+ transport channels. However, the narrow interlayer distance and the poor electrical conduction of stable 2H-MoS 2 limit its applications. In this work, the 1T-MoS 2 sheets with good electrical conduction and large interlayer spacing of 9.5 Å (designated as MoS 2 -180) have been successfully prepared by a facile hydrothermal method . The interlaminar structural water induces stable existence of metastable 1T-MoS 2 and large space distance of 6.08 Å between layers (that is larger than the size (5.5 Å) of hydrated Zn 2+ ), and contributes to its excellent hydrophilicity , promoting transmission of hydrated Zn 2+ . The interlayer spacing-tailored MoS 2 -180 cathode exhibits high specific capacity (Cs) of 226.2 mAh g −1 at 0.10 A g −1 and impressive high-rate capability. The Cs at 5.00 A g −1 is extraordinarily up to 150.9 mAh g −1 and retains 66.7% of that at 0.10 A g −1 . This is far superior to the most reported MoS 2 , MoS 2 derivatives and MoS 2 /C composite cathodes. Moreover, the activated MoS 2 -180 cathode shows robust long-term cycling stability with Cs retention of 103.6% after 500 cycles at 1.00 A g −1 . The mechanism behind these phenomena brings new insights into the structural water-induced 1T-MoS 2 for high-performance aqueous ZIBs cathodes.
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ACS Applied Energy Materials
·
2026
·
IF 5.5
Xiaorong Gan,Leilei Ye,Weiwei Wu,Kangheng Huang,Ran An,Ting Cheng,Jianlin Zhang,Yanhui Ao
Developing robust, high-performance electrochemical catalysts for hydrogen production from natural seawater or alkaline freshwater presents a significant challenge. Herein, we report an electrocatalyst system of AuCu bimetallic nanoparticles (NPs) supported on 1T-MoS2 (AuCu/1T-MoS2) synthesized via hydrothermal/solvothermal methods followed by controlled electrochemical deposition. Experimental electrochemical measurements combined with density functional theory (DFT) calculations reveal that the AuCu/1T-MoS2 catalyst exhibits superior hydrogen evolution reaction (HER) activity in alkaline freshwater compared with natural seawater. DFT indicates that adsorption of Na+ or Cl– on the active Au sites makes the Gibbs free energy of hydrogen adsorption (ΔGH) more negative, thereby disfavoring H2 desorption and reducing activity in seawater. Experimentally and theoretically, the introduction of AuCu NPs increases the density of accessible active sites by activating the otherwise inert basal planes of 1T-MoS2. The Cu component facilitates water dissociation and lowers ΔGH, while Au improves the electrical conductivity. The orbital hybridization between the d states of AuCu and those of Mo in 1T-MoS2 results in a higher density of states at the Fermi level, thereby improving conductivity and reducing ΔGH. Charge redistribution at the AuCu/1T-MoS2 interface produces a synergistic enhancement of HER kinetics. Our findings offer design principles for bimetallic/2D hybrid electrocatalysts tailored for seawater and alkaline electrolysis.
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Nano Energy
·
2022
·
IF 19.069
Sin-Yi Pang,Weng-Fu Io,Lok-Wing Wong,Jiong Zhao,Jianhua Hao
Crystal phase modulations in two-dimensional (2D) materials have garnered extensive interest because of their intriguing features and potential applications. Nonetheless, synthesizing some specific phases of metastable transition metal dichalcogenides (TMDs) remains a challenge due to the restricted selectivity under chemical and physical treatments, especially for direct growth of specific phase of TMDs on 2D substrates to form heterostructures . Taking the merits of MXene with tunable atomic vacancies and surface chemistry via surface functionalization , the phase of epitaxially grown TMDs on 2D MXene can be significantly affected. In this work, 1 T′-MoS 2 and 1 T-MoSe 2 were directly grown on electrochemically synthesized MXene under controlled oxidization conditions and selected MXene substrate. Owing to the synergistic effect of TMDs and MXene, the TMDs/MXene heterostructure catalysts exhibit good electrochemical activity under acidic conditions, with a low overpotential of 167 mV at a current density of 10 mA cm −2 . Our work not only demonstrates the distinct chemical characteristic of various MXenes feasible for surface engineering which promotes the direct and in situ growth of phase controlled TMDs on MXene substrates but also displays the high electrochemical activity in TMDs/MXene heterostructure catalysts.
研究领域:
材料科学
·
电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Lingtun Hao,Maofeng Ding,Song Song,Yong You,Xingang Li
Photocatalytic amino acid synthesis from biomass is a promising and renewable method, yet the synthesis efficiency remains suboptimal. Here, we report a novel strategy for synthesizing 2D/2D CdS/1T-MoS 2 heterojunctions by leveraging 1T-phase MoS 2 with distorted octahedral coordination and sulfur-rich edges to promote the formation of large contact areas and abundant interfacial sulfur vacancies in combination with CdS. CdS/1T-MoS 2 displays exceptional photocatalytic performance for amination of biomass-derived α-hydroxy acids to α-amino acids, achieving an alanine formation rate of 23.3 mmol·g -1 ·h -1 from lactic acid, which is 4.4 and 1.6 times higher than those of CdS and CdS/2H-MoS 2 , respectively. Detailed characterizations reveal that CdS/1T-MoS 2 possesses abundant interfacial sulfur vacancies at the 2D/2D heterojunction interface compared to CdS and CdS/2H-MoS 2 . These vacancies create numerous Lewis acids sites, significantly enhancing the adsorption and activation of hydroxyl groups in lactic acid, thereby promoting the dehydrogenation step. Moreover, CdS/1T-MoS 2 facilitates the condensation of pyruvic acid with ammonia and promotes the desorption of alanine from the catalyst surface, effectively improving the reductive amination step. Additionally, CdS/1T-MoS 2 exhibits superior charge carrier separation and migration efficiency, further boosting its photocatalytic amination activity. This study provides a novel strategy for synthesizing 2D/2D heterojunctions with abundant interfacial vacancies for efficient photocatalytic biomass valorization.
研究领域:
材料科学
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催化化学
·
生物工程
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Li-Jie He,Jia Liu,Ting-Ting Lv,Ao-Cheng Wei,Tong-Qi Yuan
The practical applications of lithium-sulfur (Li-S) batteries have severely been hindered by notorious shuttle effect and sluggish redox kinetics of lithium polysulfide intermediates (LiPSs), which bring about rapid capacity degradation, low coulombic efficiency and poor cycling stability. In this work, 1T-rich MoS 2 nanosheets are in-situ developed onto the conductive porous carbon matrix (1T-rich MoS 2 @PC) as efficient polysulfide promotors for high-performance Li-S batteries. The porous carbon skeleton tightly anchors MoS 2 nanosheets to prevent their reaggregation and ensures accessible electrical channels, and at the same time provides a favorable confined space that promotes the generation of 1T-rich MoS 2 structure. More importantly, the uniformly distributed metallic 1T-rich MoS 2 nanosheets not only affords rich sulfphilic sites and high binding energy for immobilizing LiPSs, but also favors rapid electron transfer and LiPSs conversation kinetics, substantially regulating sulfur chemistry in working cells. Consequently, the Li-S cell assembled with 1T-rich MoS 2 @PC modified separator delivers a remarkable cycling stability with ultralow capacity decay rate of 0.067% over 500 cycles at 1C. Encouragingly, under harsh conditions (high sulfur loading of 4.78 mg cm −2 and low E/S ratio of 8 μL mg −1 ), a favorable electrochemical performance can still be demonstrated. This study highlights the profitable design of 1T-rich MoS 2 /carbon based electrocatalyst for suppressing shuttle effect and promoting catalytic conversation of LiPSs, and has the potential to be applied to in other energy storage systems.
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Wenzhe Wu,Xue Ren,Chengbo Zhang,Yanqi Ding,Hengjun Gai,Meng Xiao,Quanhong Zhu,Hongbing Song,Tingting Huang
The 1T-enriched spiny-shaped nanospheres with vertically oriented MoS 2 nanosheets over the surface was successfully prepared with the novel solvent induced micelle-limited Mo-CTA + composites self-assembly (SIMMS) strategy under the dual effects of mixed sulfur sources (thiourea and thioacetamide) and cetyltrimethylammonium bromide (CTAB). In the proposed strategy, the molybdenum source and CTAB are firstly assembled to Mo-CTA + by strong electrostatic attraction to avoid the molybdenum source from polymerization and forming large polymolybdate anions. Meanwhile, the CTAB moleculars self-assemble to spherical micelles, which can adsorb Mo-CTA + through van der Waals force and obtain spherical precursors with a controllable number of nucleation sites. Under the sulfurization from mixed sulfur source, appropriate reducibility can control the formation of crystal seeds and crystal growth during the crystallization process of MoS 2 , whereas CTAB can regulate and control the growth behavior and micro-morphology of MoS 2 , which is ultimately also retained between the MoS 2 nanolayersto expand their interlayer spacing and stabilize the 1T phase. Therefore, the 1T-enriched spiny-shaped nanospheres with vertically oriented MoS 2 nanosheets can be controllably prepared. In the hydrodesulfurization (HDS) reaction of dibenzothiophene (DBT) over these catalysts, the MoS 2 -75%/0.25 catalyst with the highest concentration of sulfur vacancies as well as “rim” and “rim-like” sites can reach the highest HDS activity (99.1%) and HYD/DDS ratio (4.76), which are much higher than those of the MoS 2 -H catalyst prepared by conventional hydrothermal method (HDS DBT %=46.0%, HYD/DDS ratio=0.90).
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Nature Nanotechnology
·
2021
·Vol. 17
·期 2
·153-158
·
IF 39.213
Chen Wenshu,Gu Jiajun,Liu Qinglei,Yang Mengzhao,Zhan Cheng,Zang Xining,Pham Tuan Anh,Liu Guangxiang,Zhang Wang,Zhang Di,Dunn Bruce,Morris Wang Y.
Dense, thick, but fast-ion-conductive electrodes are critical yet challenging components of ultrafast electrochemical capacitors with high volumetric power/energy densities 1 , 2 , 3 , 4 . Here we report an exfoliation–fragmentation–restacking strategy towards thickness-adjustable (1.5‒24.0 μm) dense electrode films of restacked two-dimensional 1T-MoS 2 quantum sheets. These films bear the unique architecture of an exceptionally high density of narrow (sub-1.2 nm) and ultrashort (~6.1 nm) hydrophobic nanochannels for confinement ion transport. Among them, 14-μm-thick films tested at 2,000 mV s −1 can deliver not only a high areal capacitance of 0.63 F cm −2 but also a volumetric capacitance of 437 F cm −3 that is one order of magnitude higher than that of other electrodes. Density functional theory and ab initio molecular dynamics simulations suggest that both hydration and nanoscale channels play crucial roles in enabling ultrafast ion transport and enhanced charge storage. This work provides a versatile strategy for generating rapid ion transport channels in thick but dense films for energy storage and filtration applications.
研究领域:
材料科学
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电化学
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纳米技术
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能源存储
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高影响因子
危险品化学品经营许可证（带存储）