ENERGY & FUELS
·
2024
·
IF 5.2
Rihong Xiao,Yili Zhang,Kaiyan Long,Zhuo Xiong,Junying Zhang,Yongchun Zhao
Mercury, a toxic heavy metal, poses significant risks to human health. Coal-fired power plants are the largest anthropogenic sources of mercury emissions, making mercury removal from flue gas imperative. Among various mercury adsorbents, metal selenides show promising potential in mercury capture. Here, we reported the synthesis of a novel three-dimensional hierarchical flower-like material, SnSe2, and its debut application in flue gas mercury capture. Under the influence of low-coordinated selenium, the introduction of abundant selenium vacancy defects led to the exposure of additional active sites in the adsorbent. Additionally, the presence of Sn enhanced gas selectivity and promoted electron transfer processes, thereby augmenting Hg0 adsorption and oxidation performance. Benefiting from these advantages, SnSe2 exhibited superior mercury removal performance over a wide temperature range (30–180 °C), with a saturated mercury adsorption capacity of 2027.23 μg/g, surpassing that of commercial activated carbon. Furthermore, the presence of NO in flue gas improved mercury adsorption performance, while high concentrations of SO2 do not affect mercury removal efficiency, as elucidated by adsorption kinetics models. Moreover, the mercury adsorption mechanism was demonstrated through mercury temperature-programmed desorption (Hg-TPD) and density functional theory (DFT) calculations. Finally, toxicity characteristic leaching procedure (TCLP) experiments confirmed SnSe2 as an efficient and permanent adsorbent for mercury, offering insights into the application of novel mercury removal materials.
研究领域:
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
NANOTECHNOLOGY
·
2025
·Vol. 36
·期 13
·135402
·
IF 2.8
Yao He,Lijing Wang,Sheng Yang,Shaowei Zhang,Hongfang Du,Dandan Cui,Liangxu Lin
In lithium–sulfur batteries (LSBs), the dissolution of lithium polysulfides (LiPSs) triggers the shuttle effect to lose active materials irreversibly, leading to the fast deterioration of electrochemical performance. Rational designs on the separator membrane could mitigate the shuttle effect. However, the development of efficient separators economically remains a challenging task, aggressively limiting the commercial use of LSBs. This work reports the engineering of commercial molybdenum diselenides (MoSe2) flakes to mitigate the shuttle effect of LSBs, by forming rich Se vacancies via a potassium (K) intercalation and de-intercalation reaction. The Se vacancy in MoSex flakes significantly enhances the adsorption capacity of LiPSs and accelerates the Li+ diffusion kinetics, thereby alleviating the shuttle effect and enhancing the energy storage performance. This directly improves the energy storage performance of the LSBs by incorporating the MoSex flakes into the separator membrane, giving a high capacity retention rate of 94.6% at 2 C after 500 cycles, with a reversible specific capacity as high as 452 mAh g−1. This work offers a new strategy for the design and synthesis of vacancy rich transition metal chalcogenides for high-performance LSBs and beyond.
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
Advanced Energy Materials
·
2021
·Vol. 12
·期 1
·2102359
·
IF 29.368
Yuan Chang,Panlong Zhai,Jungang Hou,Jijun Zhao,Junfeng Gao
Faced with grave climate change and enormous energy demands, effective catalysts have become more and more important due to their significant effects on reducing fossil fuels consumption. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by water splitting are feasible ways to produce clean sustainable energy. Here, atomic structures and related scanning tunneling microscope images of Se defects in PtSe 2 are systematically explored. The equilibrium fractions of vacancies under variable conditions are predicted in detail. In addition, it is found that the vacancies are highly kinetically stable, without recovering or aggregation. The Se vacancies in PtSe 2 can dramatically enhance the HER performance, comparing to Pt(111). It is also revealed that a PtSe 2 monolayer with Se vacancies is also a good OER catalyst. The excellent bipolar catalysis of Se vacancies is further confirmed by experimental measurements. A defective PtSe 2 made via direct selenization of Pt foil at 773 K using a chemical vapor deposition process is produced. It is shown that the HER and OER performance of defective PtSe 2 is much more efficient than Pt foils by a series of measurements. This work, with its compelling theoretical and experimental studies indicates PtSe 2 with Se defects is an ideal bipolar candidate for HER and OER.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2024
·Vol. 26
·期 16
·2197-2206
·
IF 2.6
Miaomiao Wang,Weizhe Liu,Li Zhang,Huanli Liu,Xiao Yang
Transition metal selenide is a typical pseudocapacitive material used in supercapacitor electrodes, but its practical application is restricted due to its insufficient utilization rate of active sites and slow kinetics of redox reaction. Defect engineering can effectively adjust the electronic structure, provide additional intercalation sites, and realize the regulation of energy storage mechanism within the lattice. At present, heteroatom doping is an effective strategy that can provide abundant vacancy defects by introducing heterogeneous atoms, thereby achieving significantly improved electrochemical performance. Based on this, NiCo2Se4 electrode materials with Se vacancies were prepared by P doping for supercapacitors. The double-effect synergy of P doping and vacancy engineering can effectively change the electronic structure and improve the adsorption capacity of ions, which are more prone to redox reactions. The assembled hybrid supercapacitor (NiCo2Sex-P1//AC) has 90.2% capacity retention and 100% coulombic efficiency after 10 000 consecutive charge–discharge cycles, and it exhibits a high energy density of 94.6 W h kg−1 at a power density of 799.9 W kg−1. This provides an effective strategy for constructing high-performance supercapacitors.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Junfeng Qin,Qinghui Shen,Cuicui Du,Min Hong,Yixin Yang,Xiaohua Zhang,Jinhua Chen
Heteroatom doping and vacancy engineering play vital roles in designing a high-activity electrocatalyst . Herein, we proposed a novel enriched Se vacancies engineering of the promising ruthenium chalcogenide of RuSe 2 induced by low-valence Cu doping for promoting hydrogen evolution reaction (HER) electrocatalysis in alkaline media. The Cu-doped RuSe 2 with enriched Se vacancies supported on graphitized carbon (Cu-RuSe 2 @C) was synthesized by a simple one-step selenization of bimetallic MOF precursor of Ru/Cu-BTC (1,3,5-benzenetricarboxylic acid) polyhedra. Compared to the Cu(Ⅱ)-dominant doped RuSe 2 (Cu Ⅱ/Ⅰ -RuSe 2 @C) with deficient Se vacancies, the proposed Cu(Ⅰ)-dominant doped RuSe 2 (Cu Ⅰ/Ⅱ -RuSe 2 @C) with enriched Se vacancies exhibited significantly improved electrocatalytic activity, which was potentially derived from the created electron-deficient Ru δ+ and Se ν− sites induced by low-valence Cu doping. Specifically, Cu Ⅰ/Ⅱ -RuSe 2 @C needed only 40 mV overpotential to drive a HER current density of 10 mA cm −2 , comparable to commercial Pt/C (38 mV) and much lower than those of Cu Ⅱ/Ⅰ -RuSe 2 @C (93 mV) and RuSe 2 @C (362 mV). Furthermore, an alkaline Zn-H 2 O fuel cell with a Cu Ⅰ/Ⅱ -RuSe 2 @C cathode was integrated to demonstrate its potential applications, which delivered a maximum power density of 15.1 mW cm −2 and specific capacitance of 660 mAh g −1 with good stability. Two series-connected alkaline Zn-H 2 O cells acted as a chemical energy converter for simultaneous electricity generation and hydrogen coproduction by driving the coupled water splitting.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hanxiao Jia,Yuping Duan,Naibo Wu,Shude Gu,Meng Wang,Jingru Di,Jiabin Ma
The weak electromagnetic loss capability of the single semiconductor material is difficult to meet the complicated electromagnetic environment nowadays, so vacancy engineering is employed to optimize the dielectric loss capability of CoSe 2 . Selenium vacancies are introduced into CoSe 2 by re-annealing treatment, and the test results show that the selenium vacancies concentration enlarged with annealing temperature. The formation of selenium vacancies introduces a localized state in CoSe 2 , which enhances the capability of CoSe 2 to trap charge carriers, and the increased conductivity contributes to the enhancement of the dielectric loss capability. Density Functional Theory (DFT) calculations demonstrate that the selenium vacancies disrupt the original charge equilibrium distribution of the CoSe 2 , and the non-recombined positive and negative charge centers induce a strong electric dipole polarization loss. Benefiting from the optimization of CoSe 2 dielectric loss by the selenium vacancies engineering, RL min of CoSe 2 -600 reaches −30.73 dB and the effective absorption bandwidth reaches 4.00 GHz at 1.8 mm. This study provides a simple and effective solution to optimize the microwave absorption performance of single-component microwave absorption materials.
研究领域:
材料科学
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电磁学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiyang Kang,Ziqian Jin,Huaiqi Peng,Zihao Cheng,Lijie Liu,Xin Li,Lixia Xie,Jianmin Zhang,Yutao Dong
Lithium-sulfur (Li-S) batteries are currently only in the basic research stage and have not been commercialized, which is mainly affected by the poor conductivity of sulfur/lithium sulfide (S/Li 2 S), volume expansion effect of sulfur and the shuttle effect of lithium polysulfides (LiPSs). Herein, a three dimensional (3D) carbon nanotubes (CNTs) decorated cubic Co 9 Se 8−x /FeSe 2−y (0 ＜ x ＜ 8, 0 ＜ y ＜ 2) composite (Co 9 Se 8−x /FeSe 2−y @CNTs) is developed, and used as the functionalized mediator on polypropylene (PP) in Li-S batteries. Benefiting from the good electrical conductivity, large number of Se vacancies and the triple block/adsorption/catalytic effects of Co 9 Se 8−x /FeSe 2−y @CNTs, the cell with Co 9 Se 8−x /FeSe 2−y @CNTs//PP modified separator delivers a high reversible capacity (1103.5 mA h g −1 ) at 1C after three cycles activation at 0.5C and remains 446 mA g h −1 after 750 cycles with a 0.08% capacity decay rate each cycle. Moreover, at 0.2C, a high areal capacity of 3.63 mA h cm −2 after 100 cycles with a high sulfur loading of 4.1 mg cm −2 is obtained. The in-situ XRD tests revealing the transition path of α -S 8 → Li 2 S → β -S 8 during the first charge–discharge process, then β -S 8 → Li 2 S → β -S 8 conversion reaction in the next cycles, and firstly determine the sulfur-selenide active intermediates (Se 1.1 S 6.9 ) during cycles. The work provides a new insight into the development of bimetallic selenide composites by defect engineering with highly adsorptive and catalytic properties for Li-S batteries.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 35
·期 15
·2211311
·
IF 29.4
Dawei Sha,Yurong You,Rongxiang Hu,Xin Cao,Yicheng Wei,Heng Zhang,Long Pan,ZhengMing Sun
Anion vacancy engineering (AVE) is widely used to improve the Li-ion and Na-ion storage of conversion-type anode materials. However, AVE is still an emerging strategy in K-ion batteries, which are promising for large-scale energy storage. In addition, the role of anion vacancies on ion storage is far from clear, despite several proposed explanations. Herein, by employing VSe 2 as a model conversion-type anode material, Se vacancies are intentionally introduced (labeled as P-VSe 2− x ) to investigate their effect on K + storage. The P-VSe 2− x shows excellent cyclability in half cells (143 mA h g −1 at 3.0 A g −1 after 1000 cycles) and high energy density in coin-type full cells (206.8 Wh kg −1 ). By applying various electrochemical techniques, the effects of Se vacancies on the redox potentials of K-ion insertion/extraction and the K-ion diffusion in electrodes upon cycling are uncovered. In addition, the structural evolution of Se vacancies during potassiation/de-potassiation using various operando and ex characterizations is revealed. Moreover, it is demonstrated that Se vacancies can facilitate the breaking of V Se bonds upon the P-VSe 2− x conversion using theoretical calculations. This work comprehensively explains the role of anion vacancies in ion storage for developing high-performance conversion-type anode materials.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Abdelhadi El Jaouhari,Amine Slassi,Bowen Zhang,Anton Pershin,Wei Liu,David Cornil,Xiuhua Liu,Jinhua Zhu
The chemical engineering of chalcogens' defects (either selenium or sulfur) on the surfaces of Nonprecious transition metal chalcogenides provides an effective route to enhance their electrocatalytic activity . Yet, the precise role of such defects during the OER is not fully understood, which in turn precludes an efficient optimization of their catalytic activity . Herein, CoNiSe 2 film, representing a multi-transition metal selenide model with selenium defects, is electro-deposited on a carbon cloth to investigate and optimize the intrinsic and dynamic behavior of selenium vacancies during the OER process. Interestingly, the defective CoNiSe 2 with the optimized amount of selenium vacancies exhibits an advanced OER performance, including low overpotential (252 mV at 10 mA cm −2 ) and high stability for 30 h. The ex-situ XPS and Raman spectroscopies also indicate that the optimized amount of selenium vacancies can facilitate the pre-oxidation of Co and Ni sites. The latter leads to a rapid adsorption of OH − ions and a further stabilization of Co/NiOOH, which in turn mediates the efficiency of OER. The density functional theory (DFT) calculations show that the introduction of a Se-vacancy on CoNiSe 2 surface enables to adjust the changes in Gibbs free energy between different OER steps and thereby, significantly reduce the overpotential.
研究领域:
化学工程
·
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuxuan He,Jin Qian,Peifang Wang,Taiping Xie,Dionysios D. Dionysiou,Bianhe Lu,Sijing Tang
Advanced strategies for enhancing catalytic performance of catalysts include multi-metal active site exposure, vacancy growth and electronic structure optimization. Here, carbon nanotube-loaded CoSe 2 /FeSe 2 catalysts (Co/Fe-CNT) with multiphase boundaries and embedded selenium vacancies (V Se ) were prepared using a one-step hydrothermal method. The catalysts feature unique electronic structures and abundant active sites, and were found to exhibit unexpectedly high activity and stability in photocatalytic mediated sulphate radical (SR-photo) system, with impressive oxidation capacity for complex matrix polluted water. The spontaneously formed internal electric field strongly promoted charge transport and significantly enhanced the photocatalytic property. The V Se formed at the heterogeneous interface could modulate the surface electronic structure and accelerate the redox cycling of transition metals, thereby accelerating the production of reactive oxygen species and boosting the efficiency of contaminant degradation. This work provides guidance for the design of high-performance catalysts for V Se engineering and expands their potential for application in wastewater purification.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Hao Guo,Yu Liu,Henglong Ren,Yanrui Hao,Liping Peng,Wu Yang
Metal-organic framework (MOF) materials, as electrodes for supercapacitors, have promising applications, but their conductivity and capacitance performance are critical limitations to their practical use. By constructing rational structures and incorporating various active materials, the conductivity and capacitance performance of MOF-derived materials can be significantly enhanced. This study presented the application of trimetallic selenide electrode materials V a -ZnSe/NiCoSe 2 in supercapacitors prepared through sequential Ni 2 + etching, selenization and NaBH 4 reduction of ZIF-8@ZIF-67 core-shell structure. The results exhibited that an appropriate number of Se vacancy defects effectively enhanced the specific capacitance and conductivity of the material, thereby improving the performance of supercapacitors. When NaBH 4 concentration was 1 M, the obtained V 1 -ZnSe/NiCoSe 2 electrode material presented excellent supercapacitor performance with a maximum specific capacitance (capacity) of 1563 F·g −1 (705.5 C . g −1 ) at a current density of 1 A·g −1 as well as high rate capability and long-term cycling stability. Additionally, the assembled V 1 -ZnSe/NiCoSe 2 //AC asymmetric supercapacitor delivered a high energy density of 41.9 Wh·kg −1 at a power density of 750 W·kg −1 , highlighting its great potential in the field of energy storage.
研究领域:
材料科学
·
电化学
·
储能技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Wenhao Liu,Wei Li,Zhao Liang,Yufei Feng,Shaobo Ye,Chenchen Yue,Rui Ming,Xuyang Lu,Weiyou Yang,Qing Shi
The development of efficient and stable catalysts for oxygen evolution reaction (OER) is critical for the progress of electrocatalytic alkaline water and seawater hydrogen production. Herein, we report a Se-vacancy-rich Fe-doped NiSe nanosheets (VSe-FeNiSe/NFF) with remarkable OER performance in both alkaline and seawater media. It is revealed that the Se vacancies significantly promote the structural reconstruction during the OER process, which facilitates the formation of highly active NiFeOOH and SeO₄²⁻ species, thus delivering exceptional catalytic activity and stability. In alkaline media, they require an overpotential of 242 mV to achieve a current density of 100 mA cm-2, with a low Tafel slope of 27.2 mV dec-1 and robust stability over 500 h. Meanwhile, in seawater media, they just require an overpotential of 253 mV to achieve 100 mA cm-2, with a Tafel slope of 37.8 mV dec-1. Impressively, they could be operated stably for 100 h at 100 mA cm-2. This work not only elucidates the roles of Se vacancies in the reconstruction of selenides during the OER process, but also offers meaningful insight on exploring advanced electrocatalysts for OER in both alkaline water and seawater media.
研究领域:
材料科学
·
电化学
✓ 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）