JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Yanhua Lei,Jie Wang,Bochen Jiang,Hui Liu,Haifeng Lan,Yuliang Zhang,Guanhui Gao
In this study, we present the successful development of a unique photo-Fenton catalyst, 1T-2H MoS 2 @TP/PPy (MTP), achieved through the coating of a copolymer of tea polyphenol (TP) and polypyrrole (PPy) onto the surface of heterophase molybdenum disulfide (1T-2H MoS 2 ). This innovative approach involves the integration of hydrothermal synthesis with copolymerization techniques. Our strategy utilizes nanoflower-like 1T-2H MoS 2 as the foundational framework, which is then enveloped in TP and PPy copolymer. This innovative approach involves the integration of hydrothermal synthesis with copolymerization techniques. Our strategy utilizes nanoflower-like 1T-2H MoS 2 as the foundational framework, which is then enveloped in TP and PPy copolymer. This distinctive architecture demonstrates exceptional catalytic performance owing to the hetero-phase entanglement of 1T-2H MoS 2 , which provides a diverse array of active sites. The coupled structure of TP and iron (TP-Fe 2+ /Fe 3+ ) effectively overcome the limitation associated with the iron source. The incorporation of PPy not only reduces the recombination of photogenerated electron-hole pairs but also enhances the stability of 1T-2H MoS 2 . Remarkably, our experiments on the degradation of methylene blue (MB) and tetracycline (TC) degradation demonstrate that TP-Fe 2+ /Fe 3+ significantly expands the pH applicability range of the MTP composite catalyst. Additionally, we examine several factors, including different catalysts, H 2 O 2 addition, variations in light intensity, solution pH, temperature fluctuations, and the role of active species, to comprehensively understand their impact on the photo-Fenton degradation process. In conclusion, MTP composite exhibits robust catalytic stability and demonstrates a broad pH utilization range in the photo-Fenton oxidation process, highlighting its promising potential for a wide range of applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lu Zhao,Liang Liu,Xiao-Feng Bai,Ai-Yong Zhang,Shu-Chuan Peng,Chi Zhang,Hai-Hong Niu,Heng Liang
Pollutants removal by Fenton-like catalysis is of considerable interest, and the solid catalyst play governing roles. Two-dimensional MoS 2 can activate peroxymonosulfate (PMS) for radical-mediated catalysis via metallic 1T phase and/or crystal defects (i.e., sulfur vacancy). Herein, we explored the significant synergism between defective sulfur vacancy and metallic 1T rather than semiconducting 2H phase for Fenton-like catalysis on MoS 2 . This synergism was substrate-dependent during MoS 2 preparation. A series of sulfur-defected 1T-MoS 2 were prepared by H 2 O 2 oxidation, drastic structural but no morphological changes were measured. The defect-tailored 1T-MoS 2 exhibited a superior Fenton-like reactivity toward PMS activation and pollutant degradation in various water matrices. A 10.0 mg·L -1 of aqueous phenol was completely degraded in one hour, and the corresponding pseudo-first order reaction constant increased more than 12 times after defect engineering. No synergistic effect was measured between sulfur vacancy and semiconducting 2H phase on defective 2H-MoS 2 . Radical-mediated reaction mechanism was identified by ESR, scavenger inhibiting, spectroscopic analysis and electrochemical measurements. Electron transfer was accelerated within metallic 1T phase to favor PMS activation and pollutant degradation on defective sulfur vacancies serving as surface reactive sites. Our findings provided fundamental insights into PMS activation on sulfur vacancy promoted by 1T-MoS 2 in Fenton-like catalysis for water purification.
研究领域:
环境科学
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材料科学
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催化化学
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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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ENERGY
·
2025
·
IF 9.4
Ziyang Zhu,Nan He,Dong Wang,Qicheng Chen,Yingjin Zhang,Bingjian Nie
MoS 2 is considered a highly promising anode material for supercapacitors owing to its distinctive two-dimensional structure. However, its relatively low electrical conductivity restricts its further development and practical application. For the purpose of addressing this issue, this study reports the first synthesis of a CuO@MoS 2 /MXene ternary heterostructure based on hollow CuO. The formation of the built-in electric field, along with the redistribution of local charge, facilitates the transformation of 2H-MoS 2 into highly conductive 1T-MoS 2 . In addition, the three-dimensional crosslinked network structure formed by the highly conductive MXene and MoS 2 layers offers additional storage capacity for electrolyte ions, thereby further enhancing the energy storage density of the material. This negative material exhibits a maximum specific capacitance of 1435.2 F g −1 , which is significantly higher than that of most reported MoS 2 -based negative materials. The synergistic support provided by the porous CuO substrate and the MXene layer effectively inhibits the lamellar aggregation of MoS 2 , thereby achieving a capacitor retention rate of 90.1 % after 5000 charge-discharge cycles. The asymmetric supercapacitor constructed from the material achieves a maximum energy density of 91.4 Wh·kg −1 , demonstrating excellent application potential in various fields. This study addresses the research gap concerning negative electrode materials for high specific capacitance MoS 2 -based supercapacitors and offers a novel approach to further enhancing the energy density of supercapacitors.
研究领域:
材料科学
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纳米技术
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电化学
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储能技术
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无机化学
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应用物理学
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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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Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Zhang Xiankun,Liu Baishan,Gao Li,Yu Huihui,Liu Xiaozhi,Du Junli,Xiao Jiankun,Liu Yihe,Gu Lin,Liao Qingliang,Kang Zhuo,Zhang Zheng,Zhang Yue
The applications of any two-dimensional (2D) semiconductor devices cannot bypass the control of metal-semiconductor interfaces, which can be severely affected by complex Fermi pinning effects and defect states. Here, we report a near-ideal rectifier in the all-2D Schottky junctions composed of the 2D metal 1 T′-MoTe 2 and the semiconducting monolayer MoS 2 . We show that the van der Waals integration of the two 2D materials can efficiently address the severe Fermi pinning effect generated by conventional metals, leading to increased Schottky barrier height. Furthermore, by healing original atom-vacancies and reducing the intrinsic defect doping in MoS 2 , the Schottky barrier width can be effectively enlarged by 59%. The 1 T′-MoTe 2 /healed-MoS 2 rectifier exhibits a near-unity ideality factor of ~1.6, a rectifying ratio of >5 × 10 5 , and high external quantum efficiency exceeding 20%. Finally, we generalize the barrier optimization strategy to other Schottky junctions, defining an alternative solution to enhance the performance of 2D-material-based electronic devices.
研究领域:
材料科学
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纳米技术
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半导体物理
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器件工程
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Carbon Energy
·
2022
·Vol. 5
·期 2
·e255
·
IF 21.556
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
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电化学
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储能技术
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纳米技术
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电池技术
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Wang Peng,Zhao Danyang,Zhang Peng,Hui Xiaobin,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Ge Xiaoli,Liu Xiaojing,Li Yuguang C.,Yin Longwei
The metallic phase MoS 2 (1T-MoS 2 ) supported metal-nanocatalyst is an appealing material system for accelerating the redox kinetics of non-aqueous Li | |O 2 batteries. However, the drawbacks associated with the surface orbital steric effect and the internal electron coupling results in a detrimental effect for the stability of 1T-MoS 2 , especially for the interface charge transfer. This makes it difficult to incorporate guest metal nanoparticles without compromising the 1 T phase support. To circumvent these issues, here we propose a p-block element (In-O) doping strategy to stabilize the 1 T phase MoS 2 by moderating the surface orbital steric effect and strengthening the internal chemical bonding, and thus for the epitaxial Ru nanocatalyst graft on the stabilized 1T-MoS 2 for Li | |O 2 batteries. The experimental and theoretical analyzes indicate that the In-O-MoS 2 @Ru enhances the O 2 dissociation and facilitates the adsorption of LiO 2 intermediates. This effect promotes the growth of weakly crystalline Li 2 O 2 films during oxygen reduction reaction, which can be more easily decomposed during the oxygen evolution reaction, thereby enhancing the bifunctional-catalytic kinetics. When employed at the positive electrode for non-aqueous Li | |O 2 batteries, In-O-MoS 2 @Ru shows an overpotential of 0.37 V and a cycling life of 284 cycles at 200 mA g −1 with a final discharge specific capacity of 1000 mAh g −1 at 25 °C.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米技术
·
催化
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