INORGANIC CHEMISTRY
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2022
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IF 5.436
Mianmian Wu,Nan Li,Shixiang Zuo,Wenjing Shen,Guifang Sun,Qingfei Li,Minghao Shi,Jiangquan Ma
Piezocatalysis is a promising technology to address environmental pollution by converting mechanical energy into chemical energy. Herein, MoSe2 nanosheets with different 1T phase percentages (ranging from 30 to 80%) were constructed by adjusting hydrothermal temperature. Moreover, the roles of phase engineering in the piezocatalysis were thoroughly investigated by degrading rhodamine B and reducing Cr(VI) in ultrasonic vibration conditions. In particular, MoSe2 prepared at 220 °C (MoSe2-220) exhibits ultrahigh observed constant kobs and degradation rate k, which is superior to most reported catalysts to date. The experimental results indicate that the introduction of the 1T phase increases the active sites of the material, improves the conductivity, and inhibits the recombination of electrons and holes. Moreover, an internal electric field in the 2H phase induced by piezoelectric polarization is facilitated to separate electron–hole pairs, enabling the degradation and reduction to proceed. The capture experiments and EPR tests further confirm that •O2– and •OH are main reactive species, and a rational mechanism is finally put forward. This study offers a clear understanding of phase engineering in piezocatalysis and provides an efficiency strategy to construct highly efficient piezocatalysts.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
npj Quantum Materials
·
2022
·Vol. 7
·期 1
·1-8
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IF 6.856
Zhang Wenhao,Gao Jingjing,Cheng Li,Bu Kunliang,Wu Zongxiu,Fei Ying,Zheng Yuan,Wang Li,Li Fangsen,Luo Xuan,Liu Zheng,Sun Yuping,Yin Yi
The electronic evolution of doped Mott insulators has been extensively studied for decades in search of exotic physical phases. The proposed Mott insulator 1 T -TaS 2 provides an intriguing platform to study the electronic evolution via doping. Here we apply scanning tunneling microscopy (STM) to study the evolution in Ti-doped 1 T -TaS 2 at different doping levels. The doping Ti atom locally perturbs the electronic and spin state inside the doped star of David and induces a clover-shaped orbital texture at low-doping levels ( x < 0.01). The insulator to metal transition occurs around a critical point x = 0.01, in which small metallic and large insulating domains coexist. The clover-shaped orbital texture emerges at a broader energy range, revealing a competition with the electron correlation. It transforms to a disorder-induced Anderson insulating behavior as doping increases. We directly visualize the trapped electrons in d I / d V conductance maps. The comprehensive study of the series of Ti-doped 1 T -TaS 2 deepens our understanding of the electronic state evolution in a doped strong-correlated system.
研究领域:
凝聚态物理
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材料科学
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表面科学
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电子结构
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量子材料
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DOI
高影响因子
Frontiers in Environmental Science
·
2023
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IF 4.6
He Yutian,Wang Xinzhi,Ke Yuhan,Qiu Yiquan,Zhou Qiao,Shen Zheyu,Xie Han,Li Yingqiang,Huang Mingzhi
Introduction: Dimethyl phthalate (DMP) which has been widely detected in water is neurotoxic to humans and should be effectively eliminated. Persulfate-based advanced oxidation processes are considered to be reliable methods aiming at emerging contaminants degradation, while an efficient catalyst is urgently needed for the activation of the reaction. As a typical 2D material, 1T-MoS2 is expected to be applied to the activation of persulfate owing to its abundant active sites and excellent electrical conductivity. In practical applications, 1T-MoS2 has the phenomenon of reunion which affects the exposure of its catalytic sites.Methods: Therefore, in this study, we used waste cow manure as a raw material to prepare biochar and achieved high exposure of 1T-MoS2 activation sites by loading 1T-MoS2 onto the surface of cow manure biochar through hydrothermal synthesis. The prepared composite catalytic material CMB@1T-MoS2 was used to activate PMS for the degradation of DMP.Results: It was found that CMB@1T-MoS2 has better effect than CMB or 1T-MoS2 alone for the degradation of DMP, reaching 77.65% at pH = 3. Under alkaline conditions, the degradation rate of DMP was reduced due to the inhibition of the catalytic process. Among the different coexisting anions, HCO-3 interfered and inhibited the degradation process the most, leading to the lowest degradation rate of DMP with 42.45%.Discussion: The quenching experiments and EPR analysis showed that SO-4• and •OH were the main ROS in the CMB@1T-MoS2/PMS process. This study promotes the resourceful use of cow manure and is expected to provide a novel persulfate-based advanced oxidation process catalyzed by CMB@1T-MoS2 for the elimination of DMP in an aqueous environment.
研究领域:
环境科学
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催化材料
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水资源管理
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
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IF 6.182
Chao Yu,Zhanfang Cao,Shuang Chen,Shuai Wang,Hong Zhong
Designing of catalysts with high activity and earth abundance which can further enhance the electrocatalytic hydrogen evolution performance so as to improve the hydrogen production efficiency. In this paper, we synthesized 1T-MoSe 2 -Se/MgAl-LDH composites by in-situ hydrothermal reduction method. The high proportion 1T phase (73.73%) of ultra-thin layer 1T-MoSe 2 -Se was obtained by acid dissolution operation, which can be ascribed to the limiting growth effect of MgAl-LDH. Compared to Pure MoSe 2 , it dramatically improved HER catalytic activity. the optimal 1T-MoSe 2 -Se (24 h) exhibits superior HER performance with a small overpotential (122 mV at the current density of 10 mA cm −2 ) and Tafel slope (54 mV dec −1 ) as well as excellent electrochemical stability. The introduction of Se can promote the conductivity of 1T-MoSe 2 -Se catalyst. Moreover, the best electrocatalytic hydrogen evolution performance can be exhibited synergistically only when the optimal match between MoSe 2 and Se is achieved, which are confirmed by XPS analysis and HER test results.
研究领域:
材料科学
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化学工程
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能源科学
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产品关联
DOI
高影响因子
Advanced Materials Technologies
·
2025
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IF 6.2
Sheng Li,Hongcheng Ruan,Jinpeng Wang,Yuanlong Lu,Fuwei Zhuge,Tianyou Zhai
Lithium intercalation in MoS 2 drives the transformation from its semiconducting 2H to metallic 1T/1T’ phase, allowing the fabrication of low-resistance edge contacts in transistors and diodes. However, due to the presence of chemically reactive lithium, the properties of the resulting Li x MoS 2 are sensitive to processing methods, raising additional concerns about its stability and performance when applied in electronic devices, which have rarely been discussed. Here, the processing method of lithium-intercalated MoS 2 in n-butyllithium solution is investigated for optimal edge contact performance in transistors. The stability of Li x MoS 2 when exposed to various solvents, ambient environment (air and vacuum) and thermal stress (from room temperature to 300 °C) is studied in terms of its electrical conductivity and phase ratio. It is found that exposure to water causes immediate degradation of the electrical conductivity of Li x MoS 2 , while under thermal stress, irreversible degradation occurs when the temperature exceeds 150 °C. Therefore, avoiding thermal stress during device fabrication is essential. Following this, an optimal procedure is proposed to fabricate low-resistance 1T-Li x MoS 2 edge contacts, achieving a contact resistance of ≈420 Ω µm, which also displays suppressed defect states in edge-contacted transistors.
研究领域:
材料科学
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纳米电子学
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凝聚态物理
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表面科学
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半导体器件
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Jiahuang Jian,Hongjun Kang,Xianshu Qiao,Kai Cui,Yang Liu,Yang Li,Wei Qin,Xiaohong Wu
Water electrolysis is an effective method of obtaining hydrogen energy, which is the key to achieve the global “carbon neutrality” goal. Molybdenum disulfide (MoS2) with a layered structure is considered to be a competitive hydrogen evolution reaction (HER) catalyst. However, until now, metal-atom-modified 1T-phase MoS2 with rich edge active sites has rarely been reported. Herein, we first report Co and Al co-optimized 1T-phase MoS2 (CA-1T-MoS2) with rich edge active sites using a simple one-step ball-milling method. The CA-1T-MoS2 exhibits an outstanding HER performance with an overpotential value of 102 mV at 10 mA cm–2 in 1.0 M KOH. The density functional theory (DFT) results prove that the introduction of Co and Al atoms on the rich edges of 1T-MoS2 provides rich active sites, improves the electrical conductivity, accelerates the distortion of H2O to generate H* and reduces the adsorption energy of hydrogen. Thus, CA-1T-MoS2 exhibits a prominent HER performance. This work provides a novel strategy for the simple preparation of metal-atom-modified 2D transition-metal sulfide HER catalysts with rich edge active sites.
研究领域:
材料科学
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电化学
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催化
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可再生能源
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Mei Wu,Xiaohui Liang,Yu Zheng,Congyi Qian,Dunhui Wang
The core@shell structures and compositions hold greatly potential for microwave absorption. Herein, the Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures were successfully fabricated through a simple hydrothermal process. The impedance matching was significantly promoted by introducing magnetic Fe 3 O 4 nanoparticles and designing the flower-like 1 T/2 H-MoS 2 with core@shell structures. It can be seen that the regulation of Fe 3 O 4 contents play an important role in electromagnetic parameters and microwave absorption performances of the Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures. The Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures with corresponding thickness of 2.67 mm display the minimum reflection loss (RL min ) value of − 56.22 dB at 10.36 GHz (in X band), and the maximum absorption bandwidth (AB max ) extend up to 4.76 GHz with thickness of only 1.89 mm. This result is of great significance for improving microwave absorbing performance, and the nanocomposites can be regarded as candidates for high-quality absorbing materials.
研究领域:
材料科学
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电磁学
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纳米技术
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
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2025
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IF 26.8
Liming Dai,Chenchen Fang,Xiaoyuan Zhang,Yaya Wang,Rui Gao,Ying Huang,Lin Zhang,Liang Xue,Pan Xiong,Yongsheng Fu,Jingwen Sun,Junwu Zhu
The sp 3 hybridization of surface sulfur in metallic phase molybdenum disulfide (1T MoS 2 ) is identified as the intrinsic bottleneck for alkaline hydrogen production (HER), where their electron-saturated nature elevates the kinetic barrier for water dissociation. To overcome this limitation, a charge-buffered sulfidation strategy is reported to stabilize anionic boron (B δ− ) within 1T MoS 2 . By employing molybdenum aluminum boride as the precursor, the B δ− dopants can be efficiently preserved via the topological confinement imposed by Mo─B─Mo network. This approach also maintains the 1T phase integrity through Al-mediated electron compensation. Theoretical and experimental analyses reveal that B δ− substitution generates vertically oriented empty p z orbitals through sp 2 hybridization, which elevates orbital energy to align with molecular orbitals of water, significantly reducing the O─H cleavage barrier by over 80% compared to 1T MoS 2 . Concurrently, the B─Mo─S networks upshift adjacent sulfur 3p band centers to optimize the hydrogen adsorption path. These dual functionalities endow the p z -functionalized 1T MoS 2 with a low overpotential of −30 mV at 10 mA cm −2 , and high-current operation of 1 A cm −2 at 1.779 V in an anion-exchange membrane electrolytic cell. This work not only establishes orbital alignment as a transformative design principle for advanced electrocatalysts, but also paves a novel synthetic pathway for 1T transition metal disulfides.
研究领域:
电化学
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材料科学
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催化
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纳米技术
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能量转换
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 24
·13996-14003
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IF 12.732
Hongqiang Jin,Yu Yu,Qikai Shen,Peipei Li,Jia Yu,Weiming Chen,Xin Wang,Zhuo Kang,Lei Zhu,Runqing Zhao,Lirong Zheng,Weiguo Song,Changyan Cao
1T-phase molybdenum disulphide (MoS2) is considered to be one of the most promising candidates to substitute noble metals in the hydrogen evolution reaction (HER). Fabricating single layer 1T-phase MoS2 with abundant sulfur vacancies as well as good stability to further enhance catalytic performance remains a challenge. Herein, we develop an efficient in situ TMA cation ((CH3)4N+) intercalation method to produce 1T-phase MoS2. The obtained MoS2 nanosheets comprise about 81% 1T-phase and abundant sulfur vacancies (>12%), as verified by aberration-corrected high-angle annular dark field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS), etc. In addition, the surface of as-prepared ST-MoS2 is negatively charged, making it very stable in aqueous solution. The as-prepared ST-MoS2 exhibits excellent electrochemical HER performance with a low over-potential and a small Tafel slope as well as superior cycling stability. Furthermore, it is an excellent co-catalyst when coupled with CdS nanowires to form a CdS/ST-MoS2 heterojunction photocatalyst for the HER under visible light irradiation. It achieves a maximum H2 production rate and apparent quantum efficiency (AQE) of approximately 1187 μmol mg−1 h−1 and 73.4%, respectively, which are significantly higher than those of reported CdS/MoS2 photocatalysts.
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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催化
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能量转换
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jianjian Yi,Guoxiang Zhang,Xiangyang Cao,Xianglin Zhu,Li Li,Xuyu Wang,Xingwang Zhu,Yanhua Song,Hui Xu,Xiaozhi Wang
The improvement of surface reactivity in noble-metal-free cocatalysts is crucial for the development of efficient and cost-effective photocatalytic systems. However, the influence of crystallinity on catalytic efficacy has received limited attention. Herein, we report the utilization of structurally disordered MoSe 2 with abundant 1T phase as a versatile cocatalyst for photocatalytic hydrogen evolution. Using MoSe 2 /carbon nitride (CN) hybrids as a case study, it is demonstrated that amorphous MoSe 2 significantly enhances the hydrogen evolution rate of CN, achieving up to 11.37 μmol h −1 , surpassing both low crystallinity (8.24 μmol h −1 ) and high crystallinity MoSe 2 (3.86 μmol h −1 ). Experimental analysis indicates that the disordered structure of amorphous MoSe 2 , characterized by coordination-unsaturated surface sites and a rich 1T phase with abundant active sites at the basal plane, predominantly facilitates the conversion of surface-bound protons to hydrogen. Conversely, the heightened charge transfer capacity of the highly crystalline counterpart plays a minor role in enhancing practical catalytic performance. This approach is applicable for enhancing the photocatalytic hydrogen evolution performance of various semiconducting photocatalysts, including CdS, TiO 2 , and ZnIn 2 S 4 , thereby offering novel insights into the advancement of high-performance non-precious catalysts through phase engineering.
研究领域:
材料科学
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催化
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光催化
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能源材料
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Kai Wang,Nini Zhao,Haiyan Xie,Jingzhi Wang,Wenli Xu,Zhiliang Jin
Improving the separation efficiency of semiconductor photogenerated carriers is an important way to enhance the photocatalytic activity of water splitting. To establish an efficient photocatalytic hydrogen production system, a practical method combining metal-like cocatalysts with semiconductors was designed. This article prepared Ni-CdS by modifying Prussian blue analogues and synthesized Ni-CdS/1T-WS 2 composite materials by low-temperature mixing with metal-like catalyst 1T-WS 2 . At the optimal load concentration, it can reach 62.65 mmol g -1 . Firstly, the close contact interface formed between the two enables rapid transfer of photo generated electrons . Secondly, metal-like cocatalysts have a strong attraction to the charges generated by light, forcing electron hole separation and exacerbating this effect under illumination. This has been strongly demonstrated through a series of characterizations and in-situ radiation X-ray photoelectron spectroscopy. In summary, this study provides a reliable and clear understanding for the modification of Prussian blue analogues and the regulation of photo induced charge transfer by metal-like cocatalysts.
研究领域:
材料科学
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物理化学
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能源催化
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半导体光催化
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纳米材料
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 28
·12201-12207
·
IF 3.288
Yan Qiao,Xionglin Zhou,Hongchao Geng,Leilei Sun,Deshuai Zhen,Qingyun Cai
A β-NaYF4:Yb,Er,Gd nanorods@1T/2H-MoS2 nanocomposite was fabricated and used for photocatalytic sterilization under illumination from single near-infrared (NIR) light. Approximately 99.3% of Escherichia coli were killed effectively by 15 min irradiation of NIR light at a dose of 40 μg mL−1. The effective bactericidal activity is ascribed to the high upconversion luminescence efficiency of β-NaYF4:Yb,Er,Gd and the layered two-dimensional nanosheet structure of 1T/2H-MoS2. Under 980 nm light irradiation, β-NaYF4:Yb,Er,Gd emits visible light, which is absorbed by MoS2, producing strongly oxidative holes and reductive electrons. Photogenerated electron–hole pairs were able to react with H2O, O2 and OH− to produce reactive species in aqueous solution. These reactive species are strong nonselective oxidizing agents for sterilization.
研究领域:
材料科学
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纳米技术
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光催化
·
细菌学
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产品关联
DOI
高影响因子