ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Chaoqun Ma,Naihua Zhai,Bingping Liu,Shihai Yan
Although the electrochemical N 2 reduction reaction (NRR) to NH 3 provides a promising avenue for artificial N 2 fixation, building of efficient NRR electrocatalysts with high activity and stability remains a tremendous challenge. The combined experimental results and theoretical calculation reveal that MoS 2 with sulfur-vacancy defect (V S -MoS 2 ) is an admirable NRR catalyst. Electrochemical results demonstrate that V S -MoS 2 (5:2) possesses outstanding NRR performances, including a superior NH 3 average yield rate (46.1 × 10 −11 mol s −1 cm −2 at -0.5 V vs reversible hydrogen electrode (RHE)), an excellent faraday efficiency (FE: 4.58% at -0.4 V vs RHE), good electrochemical stability (at least 24 h), and high selectivity (no by-product of N 2 H 4 ). Density functional theory (DFT) calculations demonstrate that the rate determining steps (RDSs) of all V S -MoS 2 (010)-2, V S -MoS 2 (010)-1, and MoS 2 (010) are the first hydrogenation step to form *NNH intermediate, as reflected by the energy barriers of 0.06 eV, 0.20 eV, and 0.93 eV, the significantly charge transfer (1.02 e , 0.45 e vs. 0.41 e ) from two Mo atoms to N 2 , as well as the stretching of N N bond (1.200 Å, 1.140 Å vs. 0.970 Å), respectively. These results reveal that V S -MoS 2 (010)-2 can effectively activate inert N 2 molecule and have the potential application in nitrogen fixation under mild conditions.
研究领域:
材料科学
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电化学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2018
·Vol. 11
·期 13
·2130-2137
·
IF 7.411
Kai Yao,Zhanwei Xu,Zhi Li,Xinyue Liu,Xuetao Shen,Liyun Cao,Jianfeng Huang
Graphical Letting steam do the work : A grain-like MoS 2 is synthesized by sulfiding MoO 3 using a highly concentrated sulfur vapor. MoS 2 grows epitaxially on three lattice planes, giving rise to particulate MoS 2 coated with MoS 2 nanosheet. Such an architecture gives rise to good dispersity and sufficient distance between neighbors to accommodate the volume change associated with sodiation/desodiation and exhibits a high and stable capacity when used in a sodium-ion battery. MoS 2 is a promising anode material for sodium-ion batteries (SIBs) due to its attractive theoretical capacity and low cost. MoS 2 generally presents a sheet-like structure based on its (002) lattice plane; however, such a structure tends to result in agglomeration and stacking of the sheets that cannot accommodate volume expansion, resulting in poor cyclability. Herein, grain-like MoS 2 particulates (G-MoS 2 ) are synthesized by sulfiding MoO 3 in highly concentrated sulfur vapor, which results in epitaxial growth of MoS 2 in (002), (100), and (110) lattice planes, with the product consisting of MoS 2 particulates of about 300 nm coated with few-layered MoS 2 nanosheets. The unique G-MoS 2 architecture ensures good dispersion and sufficient distance to accommodate volume expansion during sodiation/desodiation, which effectively prevents stacking of MoS 2 , maintaining structural stability. When employed as the working electrode for SIB, G-MoS 2 delivers a high reversible capacity of 324 mAh g −1 at 0.5 A g −1 , retaining 312 mAh g −1 over 300 cycles with an average coulombic efficiency of 99.8 %. Even when G-MoS 2 is cycled at a high current density (2.0 A g −1 ), the retained capacity is 175 mAh g −1 after 400 cycles. Comparison with literature reveals that these capacities are among the more promising reversible values reported for pure MoS 2 .
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yiyun Wang,Xinli Li,Zhi Chen,Kai Ma,Congming Tang
This work reported the coupling reaction of lactic acid (LA) to produce pyruvic acid (PyA) and propionic acid (PA) simultaneously over defect-rich MoS2 nanosheets. The process intensification linked to dehydrogenation of LA and hydrodeoxygenation of LA brings about the advantage that is not supplied additionally with oxygen and hydrogen, achieving a green and safe route. The defected structure is characterized by high-resolution transmission electron microscopy (HRTEM) and positron annihilation lifetime spectroscopy (PALS), which promotes the catalytic performance for the coupling reaction of LA. To fully understand the importance of the defected structure, the catalytic performance of defect-free MoS2 is also evaluated. It is found that the PyA/PA ratio is less than 1 and acetaldehyde selectivity is relatively high, suggesting that the produced hydrogen from the dehydrogenation of LA is insufficient for hydrodeoxygenation of LA over defect-free MoS2, and the difference of hydrogen comes from the side reactions of decarbonylation and decarboxylation of LA. Unlike the defect-free MoS2, the dehydrogenation of LA over the defect-rich MoS2 can provide sufficient hydrogen for hydrodeoxygenation of LA, so that the side reactions are drastically weakened. The widened interplanar spacing can fully expose the defect and the LA reactant molecule is more accessible to defective sites, which can endow a better catalytic activity. Surface hydrophilicity can improve adsorption and transfer, and better activity is observed over the defect-rich MoS2 and widened defect-rich MoS2. At 300 °C and a LA LHSV of 2.6 h–1 under an inert atmosphere, the catalyst offers a satisfactory total selectivity to pyruvic acid and propionic acid of about 85%, and the molar ratio of pyruvic acid/propionic acid is 1.1.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Yanli Zhang,Jiuqing Xiong,Shihai Yan,Bingping Liu
Electrochemical reduction of nitrate to NH 3 is a very promising alternative reaction to the Haber-Bosch process, and it is necessary to develop the efficient electrocatalysts. In this study, a particle-support mode Co 3 O 4 catalyst was synthesized with ZIF-67 as the precursor, and then dispersed on MoS 2 nanoflowers by hydrothermal method. The Co 3 O 4 is anchored to MoS 2 by forming Co-S coordination bond. Furthermore, the particle-supported Co 3 O 4 exhibits better performance than Co 3 O 4 alone, as is manifested by higher Faradaic efficiencies and NH 3 yield rate at − 0.64 V (52.69% vs 32.03%; 4539.61 μg h −1 mg −1 cat vs 2048.63 μg h −1 mg −1 cat ), lower energy barriers (0.96 eV vs 1.19 eV), and better electronic conductivity (Bandwidth: 0.581 eV vs 0.613 eV). In addition, this research provides an effective solution to solve the aggregation problem of metal oxide nanoparticles.
研究领域:
化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Chengbo Wei,Chuan Liu,Linna Gao,Yanfang Sun,Qingyun Liu,Xiao Zhang,Jinxue Guo
Integrating heterogeneous hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalysts into compatible composite catalysts with specific interfaces and structures holds great promise for the development of efficient bifunctional catalysts for overall water splitting. Herein, heterogeneous MoS 2 -Ni(OH) 2 catalyst supported by Ni foam (MoS 2 @Ni(OH) 2 /NF) is developed, in which the Ni(OH) 2 nanorod array is grafted with MoS 2 nanosheets . The hierarchical 1D/2D structures benefit not only the exposure of catalytic site but also the facilitated charge transfer. The heterointerfaces allow the synergism of electric structure modulation for improved catalytic activity and kinetics towards HER, OER, and overall water splitting. MoS 2 @Ni(OH) 2 /NF achieves a current density of 10 mA cm −2 at low overpotentials of 134 and 233 mV for HER and OER in 1 M KOH, respectively. Moreover, a cell voltage as low as 1.46 V is obtained to afford 10 mA cm −2 in a tow-electrode electrolyzer using MoS 2 @Ni(OH) 2 /NF as bifunctional catalysts, assuring it superior to most of the reported noble-metal-free bifunctional electrocatalysts. Such heterogeneous design of composite catalyst should shed light on the exploration of functional materials for energy applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fengyu Tian,Wenhong Wang,Bin Liu,Yuan Pan,Bin Dong,Yichuan Li,Yanpeng Li,Hailing Guo,Yongming Chai,Chenguang Liu
The future implementation of ultralow sulfur fuel regulations requires researchers to have an excellent understanding of the mechanism of the synergistic effect between the Co(Ni) and (Mo)W sulfides in supported Co(Ni)Mo(W)S hydrodesulfurization (HDS) catalysts. This synergistic effect occurs when the distance between two metals is on the mm or nm scale. To investigate the promotion of HDS on the µm scale, a series of Co and Mo multilayer flake catalysts with a thickness of 1 mm were prepared by laminate molding. The distance between CoS x and MoS 2 in these specially structured catalysts was adjustable on the µm scale by controlling the order and quality of the catalyst powder. The results for the HDS of dibenzothiophene (DBT) demonstrate that there is an obvious synergistic effect between CoS x and MoS 2 on the µm scale. The results of pyridine IR spectroscopy indicate that this synergy is due to CoS x and MoS 2 synergistically generating more coordinatively unsaturated sites (CUSs) and -SH active sites at the μm scale, thus increasing the HDS activity. Moreover, the catalyst activity increases as the distance between CoS x and MoS 2 decreases, and the fact that the feed comes into contact with CoS x first greatly improves the activity.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Shengyu Zhou,Xiaodan Jiao,Ying Jiang,Yanan Zhao,Peng Xue,Yingshuai Liu,Jing Liu
Two-dimensional MoS 2 (2D-MoS 2 ) and its nanocomposites have been extensively studied in cancer therapy research since their prominent surface area and NIR absorption ability. In this work, Eu 3+ -incorporated MoS 2 (MoS 2 :Eu 3+ ) nanoflowers with enhanced photothermal conversion efficiency (PCE) were successfully developed by a one-step bottom-up hydrothermal method. Under 808 nm near-infrared (NIR) laser irradiation, the photothermal agents MoS 2 :5%Eu 3+ nanoflowers have a PCE at ~ 49.05%, which is 1.75 times higher than the pristine MoS 2 . MoS 2 :5%Eu 3+ as efficient photosensitizers also promote generation of cytotoxic reactive oxygen species (ROS) under 808 nm laser irradiation, thus achieving photodynamic therapy (PDT) for cancers at the same time. Enhanced in vitro breast cancer therapy through the combination of photothermal therapy (PTT) and PDT is clearly proved by using the MoS 2 :Eu 3+ nanosheet as a multifunctional nanoprobe. The unique MoS 2 :Eu 3+ works as a promising nanoprobe for PDT/PTT cancer therapies, and also provides a novel strategy for PCE improvement of the 2D-MoS 2 .
研究领域:
纳米医学
·
肿瘤学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zeyu Yuan,Junming Cao,Shulga Valerii,Hao Xu,Lili Wang,Wei Han
Sodium-ion batteries, as a promising alternative to the lithium-ion battery, have attracted extensive attention. However, due to the larger ion radius and higher standard reduction potential, the sodium-ion batteries still face poor cycle stability and relatively low energy density problems. In this work, a carbon sphere-supported Nb 2 CT x MXene/MoS 2 hierarchical structure has been designed and synthesized through hydrothermal and electrostatic self-assembly methods. The design strategy successfully improves the utilization efficiency of the MoS 2 carbon sphere as a support skeleton and reducing the diffusion path length of Na ions, leading to an improved specific capacity and rate performance. Moreover, Nb 2 CT x sheets also effectively inhibit the capacity attenuation caused by MoS 2 shedding, thus achieving the long cycle life of the sodium-ion battery. As a result, the carbon-supported MXene/MoS 2 anode delivers an ultrahigh reversible capacity, long cycling stability, and superior capacity retention rate. Notably, the carbon-supported MXene/MoS 2 anode can also obtain a considerable capacity of 196 mAh g −1 at a current density of 20 A g −1 . The full cell of SIBs was assembled, and the flexibility of the battery was tested. The density functional theory simulation results show that the sodium ion has a smaller diffusion barrier under this material design strategy.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Jiangfan Sun,Mingcai Yin,Yixian Li,Kaiyue Liang,Yaoting Fan,Zhongjun Li
CdS is a promising photocatalyst and combining MoS 2 with CdS can realize efficient photocatalytic hydrogen production. However, most of the previous researches about MoS 2 /CdS composites focus on hexagonal CdS. Studies on cubic CdS are still rare due to its unstability. Thus in this paper, a ternary composite CdS-MoS 2 /C (abbreviated as CdS-MC, M = MoS 2 , C = activated carbon) was synthesized by facile in-situ liquid phase precipitation of cubic CdS on MoS 2 /C. Based on a series of characterizations, its photocatalytic hydrogen production performance was studied. Under the irradiation of a LED lamp , a high H 2 evolution activity of 879.6 μmol h −1 was achieved for the composite CdS-10%MC, which is 23.3 times that of pure CdS. In addition, its performance is much higher than that of the hexagonal CdS-MC sample (265.6 μmol/h) obtained by heat-treatment of CdS-MC at 400 °C for 1 h under N 2 atmosphere. What’s more, the stability of CdS-MC was investigated and the possible reasons for its unstability were analyzed in detail. To improve the stability, a method of 4-mercaptobenzoic acid (4-MBA) modification was also managed. Finally, possible mechanism for the photocatalytic hydrogen production of CdS-MC was proposed.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2018
·Vol. 6
·期 3
·714-723
·
IF 4.446
Haoyang Tian,Jintao Liang,Xuli Ma,Lele Cao,Xueyan Hu,Mengting Gao,Huimin Yang,Zhenhai Liang
Graphical Photo finish : A catalyst made of MoS 2 nanosheets loaded on Cu-doped CdS nanorods is synthesized through a facile two-step solvothermal approach. The working electrode is formed by loading a certain amount of catalyst on fluorine tin oxide. A significant increase in the photoelectrochemical performance is observed, owing to the synergistic effect between CdS and MoS 2 and fast interfacial charge transfer from the Cu 2+ doping. Transition-metal ion doping and efficient decoration by using a co-catalyst have been proven to effectively inhibit the recombination of photogenerated electron-hole pairs and broaden the visible-light response region. Here, we have constructed MoS 2 nanosheets decorated on a copper-doped CdS nanorod composite as a noble-metal-free photoelectrocatalyst. This kind of composite material was constructed through a simple solvothermal method. The morphology, structure, chemical states, photoelectrochemical properties, and other properties were tested by using a diverse range of analytical techniques. Owing to the Cu 2+ doping and the excellent electron-capturing ability of MoS 2 , 5 % MoS 2 /Cu−CdS (with 7 % Cu 2+ doping in CdS) exhibits excellent hydrogen evolution reaction with a rate of 10.18 mmol h −1 g −1 , which is about 48 times higher than that of pure CdS. A significant increase in the photoelectrochemical performance of the composite catalytic material benefits from the synergistic effect between CdS and MoS 2 and fast interfacial charge transfer, owing to the Cu 2+ doping. These findings provide a new thought for further research of the ion doping in photoelectrocatalytic field.
研究领域:
材料科学
·
能源化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Wang Enze,Xiong Zixin,Chen Zekun,Xin Zeqin,Ma Huachun,Ren Hongtao,Wang Bolun,Guo Jing,Sun Yufei,Wang Xuewen,Li Chenyu,Li Xiaoyan,Liu Kai
Solitary waves are unique in nonlinear systems, but their formation and propagation in the nonlinear fluid-structure interactions have yet to be further explored. As a typical nonlinear system, the buckling of solid thin films is fundamentally related to the film-substrate interface that is further vulnerable to environments, especially when fluids exist. In this work, we report an anomalous, solitary-wave-like blister (SWLB) mode of MoS 2 thin films in a humid environment. Unlike the most common telephone-cord and web buckling deformation, the SWLB propagates forward like solitary waves that usually appear in fluids and exhibits three-dimensional expansions of the profiles during propagation. In situ mechanical, optical, and topology measurements verify the existence of an interfacial water nanolayer, which facilitates a delamination of films at the front side of the SWLB and a readhesion at the tail side owing to the water nanolayer-induced fluid-structure interaction. Furthermore, the expansion morphologies and process of the SWLB are predicted by our theoretical model based on the energy change of buckle propagation. Our work not only demonstrates the emerging SWLB mode in a solid material but also sheds light on the significance of interfacial water nanolayers to structural deformation and functional applications of thin films.
研究领域:
材料科学
·
非线性动力学
·
界面科学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 127
·期 1
·1-8
·
IF 2.584
Zhou Chenglin,Liao Gengcheng,Qiao Hui,Qi Xiang
A novel MoS 2 /Ag 2 CO 3 Z-scheme system was synthesized by a simple chemical depositing method. The morphology and material components of MoS 2 /Ag 2 CO 3 Z-scheme system were confirmed by scanning electron microscopy and Raman spectroscopy. Photoelectrochemical (PEC) tests demonstrated that the photocurrent density of MoS 2 /Ag 2 CO 3 Z-scheme system can reach up to 13 µA/cm 2 in 0.5 M Na 2 SO 4 solution at a bias voltage of 0.5 V, which is 44 times more than pure MoS 2 , as well as 13 times higher than pure Ag 2 CO 3 . Lastly, the stability measurement of MoS 2 /Ag 2 CO 3 Z-scheme system in 0.5 M Na 2 SO 4 solution was carried out showing no obvious difference after processing 50 cycles. This work demonstrates that the MoS 2 /Ag 2 CO 3 Z-scheme system may have a great potential application in photocatalytic water splitting.
研究领域:
材料科学
·
能源科学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）