Surfaces and Interfaces
·
2024
·
IF 5.7
Ziqi Zhang,Hui Yi,Jinyuan Cai,Weiguang Han,Fangyuan Zhang,Sheng-Qi Guo
Defect engineering is considered an effective means to improve the photocatalytic performance of semiconductors. However, current research on defects mainly focuses on single atom vacancies, lacking research on atomic vacancy pairs. In this work, we used SnS 2 as the research model and constructed SnS 2 nanostructures with rich S vacancies and dual S vacancy pairs, respectively. By comparing the photocatalytic activation O 2 performance of SnS 2 under different defect effects, it was found that dual S vacancy pairs have better performance optimization characteristics than S vacancies. Combining experiments and theoretical calculations, it is confirmed that dual S vacancy pairs have significant advantages over S vacancies in regulating the band structure, improving the separation efficiency of photogenerated charges and the migration rate of charge carriers, as well as activating the interface reaction of O 2 . In addition, when the catalyst is used for the removal of organic matter in water, it can be found that the optimization effect of dual defects on performance has good sustainability. This work contributes to a deeper understanding of the application scope of defect engineering and provides new ideas for the development of highly active photocatalysts.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yu Fang,Yang Cao,Bihui Tan,Qianlin Chen
Solar energy can be used as “green” energy by photocatalysis for the nitrogen fixation under the atmospheric conditions compared with the traditional energy-intensive industrial production of ammonia. However, the complex kinetics and high reaction barriers greatly hinder the development of the photocatalytic N2 reduction reaction. Herein, a BiOBr/MXene-Ti3C2 composite catalyst is prepared by the simple electrostatic adsorption and self-assembly method. The as-prepared 10 wt % BiOBr/Ti3C2 exhibits the best performance for N2 fixation to NH3 by photocatalysis. The evolution rate of NH3 is up to 234.6 μmol·g–1·h–1, which is approximately 48.8 times and 52.4 times higher than those of pure BiOBr and Ti3C2, respectively. It is found that the designed double vacancies of oxygen and titanium for BiOBr/Ti3C2 composites, with the availability of localized electrons, have the ability to adsorb and activate N2, which can be efficiently reduced to NH3 by the interfacial electrons transferred from the excited BiOBr/Ti3C2 composite. In addition, the results of in situ Fourier transform infrared show the generation of NxHy species by the continuous protonation processes. Moreover, titanium vacancy (VTi) induces a strong absorption energy for nitrogen atoms on the surface of BiOBr/Ti3C2 according to the density functional theory calculations. In particular, the P-electron feedback caused by VTi could effectively promote the weakening of the N≡N triple bond and elongate the N2 bond length by ∼31.6%. This work might provide new insights into the synergistic effect of double defects and inspiration for the rational design of catalysts by defect engineering in the field of catalytic synthesis of ammonia.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 9
·3270-3278
·
IF 6.119
Huihui Li,Fuchun Ning,Xiaofei Chen,Anye Shi
Porous carbon nitride nanosheets with carbon and nitrogen double vacancies have been synthesized by a soft template-supported one-pot method. Besides their highly defined and unambiguous structure, they also show minimal thickness and high crystallinity. This porous carbon nitride exhibits great enhancement in photocatalytic hydrogen evolution activity (297.6 μmol h−1), which is 9.6 times higher than 31.2 μmol h−1 of the pristine one. An apparent quantum yield of 12.7% at 420 nm for hydrogen production can be achieved over these porous nanosheets. The detailed investigation suggests that there are carbon vacancies along with nitrogen vacancies. Besides nitrogen vacancies, carbon vacancies also play a positive role in the improvement of hydrogen evolution. In addition, the photocatalytic performance especially hydrogen evolution increases with the increase of the C/N ratio.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Linna Dai,Xin Zhou,Yuan Yang,Pei Hu,Lijie Ci
Nonaqueous Li − O 2 battery (LOB) is considered one of the most promising energy storage system due to its ultrahigh theoretical specific capacity (3500 Wh kg −1 ). Introducing vacancies in CoMn 2 O 4 catalysts is regarded as an effective strategy to enhance the electrochemical performances of LOB. However, the relation between vacancy types in CoMn 2 O 4 and catalytic performances in the LOB remains ambiguous. Herein, ordered porous CoMn 2 O 4 with oxygen and metal vacancies is obtained via solvothermal reaction followed by temperature-controlled calcination using polystyrene spheres as templates. The increase in treatment temperature reduces the content of oxygen vacancies while increasing that of the metal vacancies. Notably, experimental results and theoretical calculations show that oxygen vacancies in CoMn 2 O 4 have a greater influence than metal vacancies in modulating the LiO 2 adsorption during the reaction processes and reducing the overpotential. CoMn 2 O 4 synthesized at 500 ℃ (CoMnO-500) with higher oxygen vacancies exhibits stronger adsorption onto the LiO 2 , facilitating the formation of film-like Li 2 O 2 . Therefore, an LOB with the CoMnO-500 catalyst presents the lowest overpotential of 1.2 V and longest cycle lifespan of 286 cycles at a current density of 200 mA g −1 . This study offers insights into the effect of CoMn 2 O 4 vacancies on the formation pathway of Li 2 O 2 discharge products.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 11
·期 1
·78-86
·
IF 3.119
Jingxuan Zheng,Bo Zhang,Zhao Wang
g-C3N4/MoS2 composites were successfully prepared by an electron-assisted strategy in one step. Dielectric barrier discharge (DBD) plasma as an electron source, which has low bulk temperature and high electron energy, can etch and modify the surface of g-C3N4/MoS2. The abundant N and S vacancies were introduced in the composites by plasma. The dual defects promoted the recombination and formation of heterojunctions of the g-C3N4/MoS2 composite. It exhibited stronger light harvesting ability and higher charge separation efficiency than that of pure g-C3N4 and MoS2. Compared with the sample by traditional calcination method, the plasma-sample showed better performance for degrading rhodamine B (RhB) and methyl orange. RhB is completely degraded within 2 hours on g-C3N4/MoS2 by plasma. A mechanism for the photocatalytic degradation of organic pollutants via the composites was proposed. An electron-assisted strategy provides a green and effective platform to achieve catalysts with improved performance.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yiyue Zhai,Xiangrong Ren,Yu Sun,Deng Li,Bolun Wang,Shengzhong (Frank) Liu
The role of multiple vacancies containing cation and anion defects in NiFe layered double hydroxide (LDH) is still worth pursuing in electrocatalytic oxygen evolution reaction (OER). Herein, a strategy integrating the oxygen and iron vacancies is proposed to fabricate NiFe LDH with highly efficient OER performance. More Fe vacancies have been introduced with increasing Fe content in NiFe-LDH structure; operando electrochemical characterizations and density functional theory (DFT) calculations reveal that the synergic effect between the iron and the oxygen vacancies promotes the generation of reconstructed active layers, optimizing the adsorption free energy of oxygen-containing intermediates. More importantly, active NiOOH intermediate species induced by oxygen vacancies are associated with OH - intercalation pseudocapacitance, activating lattice oxygen during water oxidation . The as-prepared Ni 0.3 Fe 0.7 -LDH@NF showed ultralow overpotentials of 184 and 287 mV to achieve 10 and 400 mA·cm -2 , respectively. Our work provides a new paradigm for designing high-efficiency OER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 4
·400
·
IF 4.501
Sujuan Hu,Li Jin,Wangyu Si,Baoling Wang,Mingshan Zhu
Vacancies engineering based on semiconductors is an effective method to enhance photoelectrochemical activity. Herein, we used a facile one-step solvothermal method to prepare sulfur vacancies modified ultrathin two-dimensional (2D) ZnIn2S4nanosheets. The photon-to-current efficiency of sulfur vacancies modified ultrathin 2D ZnIn2S4nanosheets is 1.82-fold than ZnIn2S4nanosheets without sulfur vacancies and 2.04-fold than multilayer ZnIn2S4. The better performances can be attributed to the introduced sulfur vacancies in ZnIn2S4, which influence the electronic structure of ZnIn2S4to absorb more visible light and act as the electrons trapping sites to suppress the recombination of photo-generated carriers. These results provide a new route to designing efficient photocatalyst by introducing sulfur vacancies.Keywords:ZnIn2S4nanosheets;sulfur vacancies;vacancies engineering;photoelectrocatalysts;photoelectrochemical performance
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jiaqi Yang,Yu Yang,Kexuan Gao,Nigel J.D. Graham,Li-an Hou
Regulation of the types and content of reactive oxygen species (ROS) in advanced oxidation processes (AOPs) is regarded as a challenging task. Herein, the features of sulfur-vacancy (Sv) and nitrogen-vacancy (Nv), and cobalt (Co)/molybdenum (Mo)-bimetallic constituents were simultaneously incorporated into a novel Co-N@MoS 2 -COOH catalyst through a simple hydrothermal calcination method. The adsorption of oxygen (O 2 ) and peroxymonosulfate (PMS) was promoted by Sv/Nv, whereby the generation of superoxide radical (O 2 · - ) and singlet oxygen ( 1 O 2 ) species was induced, and the energy barrier for the formation of high-valent cobalt-oxo species (Co(IV)=O) was reduced. The decomposition of PMS was enhanced by a bimetal (Mo/Co) electronic pump and the O 2 · - , 1 O 2 , and Co(IV)=O active species degraded tetracycline (TC) together to achieve an efficient degradation rate (initial K obs = 0.490 min -1 ). The degradation intermediates and potential degradation pathways were identified, and the leaching of Co was within the acceptable range of environmental standards. Incorporation of the catalyst into a microfilter membrane achieved a 100% degradation of TC at an ultra-high membrane flux (1803.4 LMH/bar). This study provided new insights into the types of ROS regulated by bi-vacancy and bimetallic catalysts in AOP systems, with the intention of promoting a more sustainable and resource-efficient treatment technology.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Shiming Zhang,Songyu Fan,Ting Liang,Jingwen Wei,Tingting Zhu,Yuxiang Shen,Zebin Yu,Hongxiang Zhu,Shuangfei Wang,Yanping Hou
Photocatalytic conversion of carbon dioxide (CO 2 ) into high value-added chemicals is an attractive yet challenging process, primarily due to the readily recombination of hole-electron pairs in photocatalysts. Herein, dual-oxygen-vacancy mediated Z-scheme Bi 2 Sn 2 O 7 /Sn/NiAl-layered double hydroxide (V O,O -20BSL) heterojunctions were hydrothermally synthesized and subsequently modified with Sn monomers to enhance photocatalytic activity toward CO 2 reduction. The abundance of oxygen vacancies endowed the V O,O -20BSL with extended optical adsorption, enhanced charges separation, and superior CO 2 adsorption and activation. The interfacial charges transfer of the V O,O -20BSL was demonstrated to follow a Z-scheme mechanism via photochemical deposition of metal/metal oxide. Under visible light irradiation, the V O,O -20BSL exhibited the highest yields of carbon monoxide (CO) and methane (CH 4 ), with values of 72.03 and 0.85 umol·g −1 ·h −1 , respectively, which were 2.66 and 1.57 times higher than that of the V O -NiAl-layered double hydroxide (V O -1LDH). In situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) revealed that carboxylic acid groups (COOH*) and aldehyde groups (CHO*) were the predominant intermediates during CO 2 reduction, and accordingly, possible CO 2 reduction pathways and mechanism were proposed. This study presents a feasible approach to incorporate dual vacancies into Z-scheme heterojunctions for CO 2 reduction.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Xi Hu,Yike He,Jingxiong Ma,Wenjing Dai,Yingning Zhou,Yangguang Li,Qiushi Qin,Bo Zou,Xing Li,Mingshan Wang
Tungsten disulfide (WS2) is a typical transition metal sulfide anode for sodium-ion batteries (SIBs) with multiple valence transitions and a high specific capacity. However, bulk WS2 suffers from inferior electron conductivity and a sluggish sodium-ion migration rate, severely limiting electrochemical activity. In this work, a strategy to significantly enhance the sodium-ion storage efficiency of tungsten disulfide by synergistically coupling chalcogen vacancy (sulfur and selenium) engineering with a conductive carbon network (Vc-WS2–xSex@NC) is proposed. The design approach addresses the critical limitations of bulk WS2 by introducing abundant chalcogen vacancies that act as both negative charge centers and electron carriers, thereby improving the electrochemical kinetics. Simultaneously, these chalcogen vacancies also serve as active sites to significantly contribute high levels of Na+ pseudocapacitive storage. Furthermore, the unique hybrid architecture, featuring nitrogen-doped carbon nanolayers intimately coupled with chalcogen vacancy-enriched WS2–xSex microspheres, creates a seamless and highly efficient ion/electron transport network. Thus, this design enables the Vc-WS2–xSex@NC composite to achieve an exceptional specific capacity of 328 mA h g–1 at 0.5 A g–1 in SIBs, with an impressive 94% capacity retention after 100 cycles. Moreover, the practical applicability of this material is demonstrated through the assembly of a full cell (Vc-WS2–xSex@NC||Na3V2(PO4)3), which exhibits a remarkable reversible capacity retention of 87% after 100 cycles at 0.5 A g–1.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Gang Yang,Yan Yang,Yan Li,Fangxiang Song,Qianlin Chen
Lower voltage window and limited pseudocapacitive active sites are identified as critical impediments hindering the advancement of nickel-based supercapacitors. Herein, a double-confined strategy involving nanosizing and heterointerfaces is proposed to construct nickel-based sulfide composite (PMO@NiS 2 /Ni 0.96 S@C) with abundant oxygen vacancies (O V ), sulfur vacancies (S V ), and heterostructures. The composite was prepared using liquid-phase in situ self-assembly and low-temperature in situ induction techniques. The double-confined structure and the introduction of vacancies can effectively expose the pseudocapacitive active sites and improve the operating voltage window range of nickel nanosulfides to enhance pseudocapacitive performance. It is determined that anions and cations in the electrolyte are collectively implicated in the energy storage process. Meanwhile, electrochemical quasi-in situ XPS, in situ electrochemical quartz crystal microbalance (EQCM), and theoretical calculations based on density functional theory (DFT) were utilized to verify the energy storage mechanisms of anions and cations in the electrolyte. Furthermore, a pseudocapacitive reaction mechanism for the composites is proposed, which encompasses a novel charge storage coupling effect between the surface redox reaction of the electrolyte anions and the intercalation/de-intercalation of the electrolyte cations at the interlayer and heterointerface. Consequently, the (PMO@NiS 2 /Ni 0.96 S@C) electrode achieves 1807 C/g (6 M KOH, 0.25 A/g) under the working potential window of −0.8 ∼ 0.5 V. The assembled symmetric supercapacitor demonstrates a specific potential of 2 V, yielding an energy density of 96 Wh kg −1 at a power density of 300 W kg −1 . This work provides a theoretical reference for designing nickel-based compound materials with high energy density.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hui-xin Wang,Hui Ren,Liu Yin,Ya-ru Li,Xin-zhou Wu
Boron has a high calorific value and good application prospects in energetic materials. However, further applications of boron are hindered by its incomplete combustion. MoO 3 has good catalytic properties, and its layered structure can provide good ion flow channels and embedding positions. In this study, mechanical mixtures of B/MoO 3 and B/Mo were prepared. The promotion of B combustion by MoO 3 and Mo was confirmed via combustion heat and burning rate tests. The mechanism by which Mo/MoO 3 promote B combustion was studied by thermal analysis, high-temperature in situ X-ray diffraction, X-ray photoelectron spectroscopy, and Raman spectroscopy . The maximum heat release and burning rate of B/MoO 3 and B/Mo were 2.49 and 2.62 and 2.67 and 2.55 times, respectively, those of raw boron. A pre-ignition reaction occurred when boron first came into contact with the surface of MoO 3 . The oxygen vacancies on the MoO 3 surface served as reaction sites for boron. MoO 3 promoted the combustion of B by opening up oxygen channels and improving the oxygen transport capability. Mo also effectively promoted boron combustion. B/Mo and B/MoO 3 have promising future applications as high energy release materials.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）