ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chunlei Wang,Chunyu Zhao,Xiangjun Pu,Yubin Zeng,Yingjin Wei,Yuliang Cao,Zhongxue Chen
Aqueous zinc-ion batteries (ZIBs) are competitive among the elective candidates for electrochemical energy storage systems, but the intrinsic drawbacks of zinc metal anodes such as dendrites and corrosion severely hinder their large-scale application. Developing alternative anode materials capable of high reversibility and stability for storing Zn2+ ions is a feasible approach to circumvent the challenge. Herein, a sulfur-defect-induced TiS1.94 (D-TiS1.94) as a promising intercalation anode material for ZIBs is designed. The abundant Zn2+-storage active sites and lower Zn2+ migration barrier induced by sulfur defects endow D-TiS1.94 with a high capacity for Zn2+-storage (219.1 mA h g–1 at 0.05 A g–1) and outstanding rate capability (107.3 mA h g–1 at 5 A g–1). In addition, a slight volume change of 8.1% is identified upon Zn2+ storage, which favors a prolonged cycling life (50.3% capacity remaining in 1500 cycles). More significantly, the D-TiS1.94||ZnxMnO2 full battery demonstrates a high discharge capacity of 155.7 mA h g–1 with a capacity retention of 59.8% in 400 cycles. It has been estimated that the high-capacity, low-operation voltage, and long-life D-TiS1.94 can be a promising component of the ZIB anode material family, and the strategy proposed in this work will provide guidance to the defect engineering of high-performance electrode materials toward energy storage applications.
研究领域:
材料科学
·
电化学能存储
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DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Jiaxin Song,Cheng Rao,Zeshu Zhang,Xiangguang Yang,Yibo Zhang
Photocatalytic reforming of plastics, involving converting plastics into valuable chemicals while producing hydrogen from water, is a promising green technology with sustainability potential. However, designing catalysts with optimized structures to further enhance efficiency remained a major challenge. In this study, a series of CdS Quantum dots (QDs) with different sulfur defect concentrations were synthesized by a one-step solvothermal method by adjusting the type of sulfur precursors. In the absence of co-catalysts, the optimal CdS-NS photocatalyst achieved reforming of polyethylene terephthalate (PET) into formate with 870 μmol g −1 h −1 and acetate esters with 90 μmol g −1 h −1 , while the hydrogen production rate reached 1771 μmol g −1 h −1 . EPR spectra and other analyses confirmed the presence of abundant sulfur defects in the prepared CdS QDs and further demonstrated that the concentration of sulfur defects was closely related to photocatalytic performance. Suitable sulfur defects effectively modulated the electronic and band structure of CdS QDs, enhanced the oxidation capacity of photogenerated holes, reduced the recombination rate of charge carriers, and ultimately improved photocatalytic activity. This work provided an effective approach for designing efficient photocatalysts for the high-value recycling of plastic waste to achieve carbon neutrality.
研究领域:
材料科学
·
环境科学
·
化学工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Jun Cai,Yi Xia,Ruiqi Gang,Sufang He,Sridhar Komarneni
Defect engineering and heterogeneous doping are considered as the effective routes to improve the photocatalytic activity of MoS 2 . In this study, tungsten was used to produce sulfur defects and tungsten doping on MoS 2 by one step hydrothermal treatment. Tungsten doping not only promotes the formation of sulfur defects, but also accelerates the efficiency of separation and transfer of electron-hole pairs, which enables the samples to maintain high catalytic oxidation activity for a long time. Furthermore, comparative experiments show that sulfur defects can promote the activation of O 2 and the formation of more active O 2 - and ·OH species. As a result, the W-doped MoS 2 exhibited a high removal efficiency of more than 99% of gaseous mercury. In addition, W-doped MoS 2 showed good stability, long term durability, enhanced water and sulfur resistance under light illumination. This work provides a novel direction for designing efficient photocatalysts based on transition metal dichalcogenides.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 60
·90248-90258
·
IF 5.19
Zhang Qian,Zhou Jinwen,Zhang Lishan,Zhong Shan,Ru Xuan,Shu Xiaohua
Pyrite affects the adsorption of tylosin (TYL) due to their coexistence in the lake system. As well as the reactivity groups of S–S-H, S-OH, and Fe-OH, defects also have the possibilities to influence the adsorption of organic contaminants. However, the role of these active sites in antibiotic adsorption on pyrite has not been deeply studied. Besides, pH, N, P, dissolved oxygen, and dissolved organic matter (DOM) fluctuate greatly in lake at different seasons, which may change the surface characteristics of pyrite. Hence, the adsorption of TYL on natural pyrite considered solution chemistry and DOM in lake water was explored in this study. The fitting results of the kinetic and isotherm models showed that the adsorption included physical and chemical interactions. The neutral initial solution pH was conductive to TYL adsorption owing to the combined result of electrostatic and cover of Fe-oxyhydroxide. NO 3 − and NH 4 + had no effect on TYL adsorption, whereas H 2 PO 4 − promoted adsorption by forming flocculent Fe(H 2 PO 4 ) 3 precipitates. The dissolved oxygen increased adsorption. This is due to the co-promotion of the pyrite oxidation by oxygen and sulfur defects. The Fe(II)-DOM complex caused by pyrite surface oxidation reduced the concentration of TYL in solution by gathering. Except for the surface charge, reactivity groups on pyrite significantly influenced the adsorption of TYL. The bond fracture of S–S resulted in sulfur defects that contributed to pyrite oxidation. As a result, Fe(III)/Fe(II) on the surface of pyrite or in solution produced a complex Fe(III)/Fe(II) with anions and DOM. In addition, Fe(III)-S on sulfur defects interacted with the O–H of TYL through hydrogen bonding. Furthermore, the Fe–O-C bond is formed by the interaction of C–OH on TYL and Fe(III) (hydr)oxides on the surface of pyrite. The study provides a deep insight into the effect of pyrite surface active sites on amphoteric antibiotic adsorption. It helps to understand antibiotic migration and interactions with widespread pyrite in the real environment. Graphical abstract
研究领域:
环境科学
·
水文学
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DOI
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 48
·485403
·
IF 3.953
Martine Otay Lifoka,Weixing Niu,Guihua Liu,Changcheng Wu,Jingde Li
Non-precious and stable electrocatalysts towards both oxygen and hydrogen evolution reaction (OER/HER) are essential for effective overall water splitting in alkaline solution. In this study, a sulfur defective and manganese-doped nickel sulfide nanosheet that uniformly grown on nickel foam substrate (Mn–Ni3S2–x@NF) is synthesized. In alkaline solution, the Mn–Ni3S2–x@NF showed a low overpotential of 76 and 110 mV for OER and HER at 10 mA cm−2, respectively, together exhibiting excellent stability for both OER and HER reaction. It was confirmed by the experimental results that sulfur defects and Mn-doping synergistically optimized the electronic structure of Mn–Ni3S2–x with increased electrical conductivity and enhanced OER/HER activity. Moreover, amorphous nickel oxyhydroxide (NiOOH) was observed by in situ Raman during the OER condition, suggesting NiOOH is the active phase for OER reaction. Furthermore, the electrolyzer assembled by Mn–Ni3S2–x@NF merely needs 1.46 V to reach 10 mA cm−2 and shows good stability as well. This study provides a feasible way to prepare high-efficiency bifunctional catalysts for overall water splitting.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2019
·Vol. 12
·期 3
·1958-1966
·
IF 6.97
Peng Yang,Yabing Shan,Jing Chen,Garel Ekoya,Jinkun Han,Zhi-Jun Qiu,Junjie Sun,Fei Chen,Haomin Wang,Wenzhong Bao,Laigui Hu,Rong-Jun Zhang,Ran Liu,Chunxiao Cong
Monolayer MoS2 is a direct bandgap semiconductor which is believed to be one of the most promising candidates for optoelectronic devices. Chemical vapor deposition (CVD) is the most popular method to synthesize monolayer MoS2 with a large area. However, many defects are always found in monolayer MoS2 grown by CVD, such as sulfur vacancies, which severely degrade the performance of devices. This work demonstrates a concise and effective method for direct growth of high quality monolayer MoS2 by using SiO2/Si substrates pretreated with sulfur vapor. The MoS2 monolayer obtained using this method shows about 20 times PL intensity enhancement and a much narrower PL peak width than that grown on untreated substrates. Detailed characterization studies reveal that MoS2 grown on sulfur vapor pretreated SiO2/Si substrates has a much lower density of sulfur vacancies. The synthesis of monolayer MoS2 with high optical quality and low defect concentration is critical for both fundamental physics studies and potential practical device applications in the atomically thin limit.
研究领域:
材料科学
·
光学
·
半导体物理
✓ 已验证
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Xuedong Jing,Na Lu,Jindou Huang,Peng Zhang,Zhenyi Zhang
Engineering lattice defects in two-dimensional (2D) sulfide semiconductors has been accepted as an effective strategy to enhance the efficiency of the solar-to-fuels conversion. Although many researches have proven the lattice defect-mediated photocatalytic activity of ZnIn 2 S 4 , the artificial control of S-defects for optimizing the charge-carrier kinetics process in ZnIn 2 S 4 has long been a challenging task. Herein, we report a facile one-step method to modulate the lattice S-content of ZnIn 2 S 4 microflowers (MFs) only through adjusting the used amount of S-precursor in the hydrothermal solution that contains the metal precursors with a fixed Zn/In stoichiometric ratio at 1:2. We also demonstrated that the S-vacancies at the In facets were the main type of lattice defects in the formed ZnIn 2 S 4 MFs, which could enhance both the separation and migration processes of the photoinduced charge-carriers due to the existence of discrete defect energy-levels (DELs) and the reduced effective mass of electrons, as evidenced by the first-principles calculations and the electron spectra analyses. The ZnIn 2 S 4 MFs with the optimal content of S-vacancy obtained by a hydrothermal treatment of the precursors with the Zn/In/S stoichiometric ratio of 1:2:8 possessed the long-lived photoinduced electron (~94.64 ns) for contributing to the photo-physical and -chemical processes. Thus, upon visible light irradiation, the H 2 -evolution rate of this sample reached ~ 2.40 mmol h −1 g −1 with an apparent quantum efficiency of ~ 0.16% at 420 nm even though only using 5 mg of photocatalysts without any cocatalysts .
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2021
·Vol. 8
·期 7
·2069-2080
·
IF 8.131
Xuan He,Lei Zhang,Xiangang Hu,Qixing Zhou
Solar steam generation has attracted interest in water purification and seawater desalination as an efficient solar energy conversion method. However, the complex preparation process and limited efficiency restrict the practical applications of solar-generated steam. Here, we report a three-dimensional wood membrane inside coated with MoS2 (WM-H, with S defects) for efficient seawater desalination. The vertically aligned mesoporous wood channels and their inner microstructures increase the contact interface between water and MoS2 in wood. The formation of S defects allows the surface temperature of the membrane to reach ∼53 °C under 1 sun illumination. The MoS2-coated wood with S defects exhibited an excellent evaporation flux (1.46 kg m−2 h−1, one sun), with a solar thermal conversion efficiency of 82.5%. The adsorption peak values of Na+ on the two sides of MoS2 with defects are 2.17 times and 1.49 times higher than those of MoS2 without defects. The wood-based design provides an inexpensive way to capture solar energy and generate steam.
研究领域:
材料科学
·
能源工程
·
环境科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hongbin He,Xuan Jian,Tianxu Zen,Bingbing Feng,Yanan Hu,Zhongqiang Yuan,Zizhen Zhao,Xiaoming Gao,Lei Lv,Zhenheng Cao
The rapid recombination of interfacial charges is considered to be the main obstacle limiting the photocatalytic CO 2 reduction. Thus, it is a challenge to research an accurate and stable charge transfer control strategy. MIL-53 (Al)-S/Cd 0.3 Zn 0.7 S (MAS/CZS-0.3) photocatalysts with chemically bonded interfaces were constructed by in-situ electrostatic assembly of sulfur defect Cd 0.3 Zn 0.7 S (CZS-0.3) on the surface of MIL-53 (Al) (MAW), which enhanced interfacial coupling and accelerated electron transfer efficiency. An adjustable proportion of syngas (H 2 /CO) was prepared by photothermal catalytic CO 2 reduction at micro-interface. and the optimal yield of CO (66.10 μmol∙g −1 ∙h −1 ) and H 2 (71.0 μmol∙g −1 ∙h −1 ) was realized by the MAS/CZS-0.3 photocatalyst. The improved activity was due to the photogenerated electrons migrated from CZS-0.3 to the adsorption active sites of MAS , which strengthened the adsorption and activation of CO 2 on MAS. The photothermal catalytic CO 2 reduction to CO follows the pathway of CO 2 →*COOH → CO and CO 2 →*HCO 3 – →CO. This work provided a reference for the research, characterization, and application of in-situ anchoring of metal organic frameworks in photothermal catalytic CO 2 reduction, and provided a green path for the supply of Syngas in industry.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yaoyao Wu,Xiaotao Chen,Jiachun Cao,Yuqing Zhu,Wenjing Yuan,Zhuofeng Hu,Zhimin Ao,Gary W. Brudvig,Fenghui Tian,Jimmy C. Yu,Chuanhao Li
Photocatalysis is a promising technology for energy and environment applications. Herein, a dual-defect heterojunction system of TiO 2 hierarchical microspheres with oxygen vacancies modified with ultrathin MoS 2−x nanosheets (MoS 2−x @TiO 2 -OV) is designed for simultaneously degrading pollutants and evolving hydrogen. MoS 2−x @TiO 2 -OV exhibits a dramatically enhanced photocatalytic activity with a H 2 evolution rate of 2985.16 μmol g −1 h −1 . In treating the simulated pharmaceutical wastewater, MoS 2−x @TiO 2 -OV is capable of purifying various refractory contaminants, with the highest H 2 evolution rate of 41.59 μmol g −1 h −1 during enrofloxacin degradation. While treating the simulated coking wastewater, the catalyst achieves a H 2 evolution rate of 102.72 μmol g −1 h −1 and a mineralization rate of 50%. Computational studies suggest that the dual-defect is superior for the adsorption of H* and producing·OH (‘dual-defect boosted dual-function’). Also, the dual-defect sites significantly boosted the charge-carrier separation and transfer efficiencies. This work highlights the crucial role of defect engineering to develop the energy-recovering wastewater treatment approaches.
研究领域:
环境科学
·
材料科学
·
化学工程
·
能源化学
·
光催化
·
水污染控制
·
纳米材料
·
可持续能源
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiangyu Li,Mengyuan Yu,Ying Han,Ning Fu,Lian Qin,Jie He,Zhongli Zhao,Guixiang Teng,Chun Zhang
Guided by the principles of active site exposure and electron transport kinetics, we innovatively constructed a porous carbon sphere photocatalyst loaded with sulfur-deficient bimetallic sulfides C/Sv-CuIn 5 S 8 through a high-temperature calcination-induced vacancy strategy. By constructing a triple platform that integrates a hollow carbon sphere substrate, a bimetallic synergistic effect, and controllable sulfur defect states, the catalyst maximizes the efficiency of the entire CO 2 adsorption-activation-conversion chain, thereby exhibiting exceptional photocatalytic activity. Compared with pure CuIn 5 S 8 , the CH 4 and C 2 H 6 production in C/Sv-CuIn 5 S 8 increased significantly from 17.2 ± 0.5 μmol g −1 and 7.9 ± 0.5 μmol g −1 to 74.7 ± 0.4 μmol g −1 and 28.4 ± 0.6 μmol g −1 , with the increase rates reaching 4.4 times and 3.6 times respectively, while also possessing superior stability (activity retention >90 % after 6 cycles). In-situ infrared spectroscopy and density functional theory calculations have elucidated its reaction mechanism, revealing that sulfur vacancies alter the reaction pathway: On C/Sv-CuIn 5 S 8 , the formation of the key intermediate HCOO* is nearly spontaneous with an energy barrier of −0.63 eV, thereby effectively suppressing the generation of CO. it is further inferred that the formation of C 2 H 6 originates from the C C coupling of two CH 3 intermediates, while some of the uncoupled *CH 3 are protonated, leading to the high yield of CH 4 . This study provides a reference for the application of bimetallic sulfide carbon-based composite materials in the photocatalytic reduction of CO 2 .
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Nianqi Meng,Peijing Xu,Changchun Wen,Huihui Liu,Cunji Gao,Xing-Can Shen,Hong Liang
Bismuth sulfide is widely used as an n -type semiconductor material in photocatalytic reactions. However, bismuth sulfide has poor absorption in the near-infrared region and low charge separation efficiency, limiting its application in phototherapy and sonodynamic therapy (SDT). In this study, we successfully synthesized an “all-in-one” phototheranostic nanoplatform, namely Bi 2 S 3-x [email protected] , based on a single second near-infrared (NIR-II) light-responsive Schottky-type Bi 2 S 3-x -Au heterostructure for photoacoustic (PA) imaging-guided SDT-enhanced photodynamic therapy (PDT)/photothermal therapy (PTT). Bi 2 S 3-x [email protected] exhibits excellent NIR-II plasmonic and photothermal properties, rendering it with NIR-II PA imaging capabilities for accurate diagnosis. Additionally, the high-density sulfur vacancies constructed on the Bi 2 S 3 surface cause it to possess a reduced band gap (1.21 eV) that can act as an electron trap. Using the density functional theory, we confirmed that the light and ultrasound-induced electrons are more likely to aggregate on the Au nanoparticle surface through interfacial self-assembly, which promotes electron-hole separation and enhances photocatalytic activity with increased reactive oxygen species (ROS) generation. With a further modification of hyaluronic acid (HA), Bi 2 S 3-x [email protected] can selectively target cancer cells through HA and CD44 protein interactions. Both in vitro and in vivo experiments demonstrated that Bi 2 S 3-x [email protected] effectively suppressed tumor growth through SDT-enhanced PTT/PDT under a single NIR-II laser and ultrasound irradiation with negligible toxicity. Our findings provide a framework for fabricating Schottky-type heterostructures as single NIR-II light-responsive nanotheranostic agents for PA imaging-guided cancer phototherapy.
研究领域:
生物医学工程
·
纳米技术
·
癌症治疗
·
材料科学
·
医学成像
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）