FUEL
·
2024
·
IF 6.7
Qitong Xue,Jiaying Xing,Jianjun Chen,Jinxing Mi,Jianqiang Shi,Yao Wang,Junhua Li,Zhiming Liu
V 2 O 5 /TiO 2 has been wide used in the selective catalytic reduction of NO x by NH 3 (NH 3 -SCR). However, the poisoning mechanism of thallium (Tl) on the catalytic performance of commercial V 2 O 5 /TiO 2 catalyst has remained unclear. Herein, we have systematically investigated the poisoning effect of Tl based on the different characterizations and DFT calculations. It was found that the strong interaction between V and Tl exists, resulting in the transformation of V from monomeric VO x to polymeric and crystalline VO x , the formation of V-O-Tl species, a decrease in the active V 5+ sites, and the inhibition of the adsorption and activation of NH 3 on both Brønsted and Lewis acid sites. Mechanistic studies further confirmed that inactive nitrate intermediate species gradually accumulated over V 2 O 5 /TiO 2 catalyst surface due to the presence of Tl. A combination of factors ultimately led to the deactivation of the V 2 O 5 /TiO 2 catalyst. This study unveils the poisoning mechanism of Tl on V-based catalysts and shed light on the design of Tl-tolerant NH 3 -SCR catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2022
·
IF 6.796
Zhihui Lv,Guangzhi He,Wenshuo Zhang,Jingjing Liu,Zhihua Lian,Yang Yang,Zidi Yan,Guangyan Xu,Wenpo Shan,Yunbo Yu,Hong He
TiO 2 -supported V 2 O 5 catalysts are commonly used in NO x reduction with ammonia due to their robust catalytic performance. Over these catalysts, it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities, namely the interface sites. To reveal the role of V-O-Ti entities in NH 3 -SCR, herein, we prepared TiO 2 /V 2 O 5 catalysts and demonstrated that V-O-Ti entities were more active for NO x reduction under wet conditions than the V sites (V=O) working alone. On the V-O-Ti entities, kinetic measurements and first principles calculations revealed that NH 3 activation exhibited a much lower energy barrier than that on V=O sites. Under wet conditions, the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH 3 activation. Under wet conditions, meanwhile, the migration of NH 4 + from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic; thus, V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH 3 pool and active centers for activation of NH 4 + . This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO x removal under realistic conditions, providing a new perspective on NH 3 -SCR mechanism.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2025
·
IF 14.1
Hai Zhu,Tinghua Li,Xinhao Peng,Xiaoxian Zhang,Xuequan Zhang,Qiusheng Wang,Lei Lei,Jun Zhang,Bin He,Jun Cao
MXenzymes, a promising class of catalytic therapeutic material, offer great potential for tumor treatment, but they encounter significant obstacles due to suboptimal catalytic efficiency and kinetics in the tumor microenvironment (TME). Herein, this study draws inspiration from the electronic structure of transition metal vanadium, proposing the leverage of TME specific-features to induce structural transformations in sheet-like vanadium carbide MXenzymes (TVMz). These transformations trigger cascading catalytic reactions that amplify oxidative stress, thereby significantly enhancing multimodal tumor therapy. Specifically, the engineered HTVMz, coated with hyaluronic acid, exhibits good stability and generates a thermal effect under NIR-II laser irradiation. The thermal effect, combined with TME characteristics, facilities a structural transformation into ultra-small vanadium oxide nanozymes (VO x ). The enlarged surface area of VO x substantially enhances ROS regeneration and amplifies oxidative stress, which promotes lysosomal permeability and induces endoplasmic reticulum stress. The high-valent vanadium in VO x interacts with intracellular glutathione, disrupting redox homeostasis and intensifying oxidative stress further. These amplifications accelerate tumor apoptosis, induce ferroptosis, and suppress HSP90 expression. Consequently, the heightened thermal sensitivity of HTVMz synergistically promotes tumor cell death via multimodal therapeutic pathways. This study presents an innovative strategy for tumor catalytic therapy by manipulating MXenzymes structures, advancing the field of catalytic therapy.
研究领域:
生物医学工程
·
肿瘤学
·
纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ziwei Gan,Xiaohe Ren,Mingdong Liu,Nengze Wang,Tianning Pian,Mengxuan Sun,Chunyang Jia,Zhijie Li
Layered vanadium-based materials are considered to be the most promising cathode materials for aqueous zinc ion batteries (AZIBs) due to their abundant valence changes and high theoretical capacity. However, low intrinsic conductivity, poor low temperature performance and generally poor cycle life hinder their further application. This study proposes a 3D conductive network by compositing vanadium-based materials with graphene to improve the conductivity for rapid electron transfer. Meanwhile, the interleaving of vanadium-based materials with the conductive network of graphene constructs a buffer layer, which can effectively mitigate the structural collapse caused by Zn 2+ insertion/extraction during the charge and discharge processes, and significantly increase the long cycle life of the battery. The H 2 V 3 O 8 /rGO conductive network buffer layer is directly synthesized by a one-step hydrothermal method. The H 2 V 3 O 8 /rGO-100//Zn batteries show a specific capacity of up to 528.3 mAh/g at 0.1 A/g. Even at a high working current density of 20 A/g, the specific capacity is still 137.2 mAh/g, and it can remain 88.8 % after 12,000 cycles. Moreover, at the low temperature of −20 °C, the H 2 V 3 O 8 /rGO-100//Zn still maintain a high specific capacity of 346.6 mAh/g at 0.1 A/g, and its specific capacity can remain 86.2 % after 20,000 cycles at 10 A/g. Even at −30 °C, it can stably work for 3,000 cycles at 1 A/g with almost no capacity degradation, showing good low temperature adaptability. Therefore, the present work provides a novelty strategy of designing cathode materials for ZIBs with excellent performance.
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
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Lei Chen,Jin-Tao Ren,Zhong-Yong Yuan
The modification of electronic structure in heterogeneous catalysts has been particularly proven as one of efficient approaches for enhancing the catalytic performances in redox. Herein, phosphorus-doped g-C 3 N 4 nanosheets with atomically dispersed V-based nanocomposites (V/P-CN) were fabricated through a facile organophosphonic acid-modified co-condensation route. The use of organophosphonic acid not only achieves the in-situ P-doping but also tailors the texture of the synthesized V/P-CN, leading to narrow band gap, electron-enriched structure, nanosheet morphology, abundant mesh-like pores and enlarged surface area. Series of physicochemical and electrochemical characterizations indicate the enhanced electron transfer from the P-doped g-C 3 N 4 to V-based nanocomposites. The heterojunction-induced electron–enriched structure of V-based nanocomposites in V/P-CN endows with the impressive intrinsic oxidative desulfurization activities. Radical scavenger experiment further suggests the significant electron interaction in the heterojunction catalysts favors the enriched electron dispersion around V-based active species and employs as rate-determining step for oxidative desulfurization. This work offers a facile but economic and powerful method to modulate the structure of the heterojunction catalysts for green catalysis, especially redox reactions.
研究领域:
催化化学
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材料科学
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Jiaying Xing,Qitong Xue,Jianjun Chen,Jinxing Mi,Xiaoping Chen,Jianqiang Shi,Zhiming Liu,Junhua Li
Vanadium-based catalysts play a pivotal role in the emission control of industrial NOx via selective catalytic reduction (SCR) technology. However, little attention has been paid to the potential emission of greenhouse gas N2O under complex working conditions. This work reports that a commercial V2O5/TiO2 catalyst may lead to significant N2O emission without greatly changing the outlet NOx concentration after chromium (Cr) deposition. With a Cr loading of 2 wt %, N2O concentration increased from 27.8 to 199.2 ppm at 350 °C with the value of outlet N2O/(N2O+N2) from 2.5% to 19.4%. Experimental results combined with DFT+U calculations suggest that nonselective catalytic reduction (NSCR) is the main route for N2O formation in a wide temperature range of 250 ∼ 400 °C. It is stemmed from the fact that the covalent interaction between Cr and V species on the V2O5/TiO2 surface accelerates the conversion of V4+ + Cr6+ → V5+ + Cr3+, leading to a larger proportion of surface V5+. More importantly, surface V5+ is highly related to the redox property of the V2O5/TiO2 catalyst, which is beneficial to NSCR reaction rather than the standard SCR process. The work suggests that to better inhibit the emission of greenhouse gases during the NH3–SCR process, monitoring N2O emission should be included along with the NOx concentrations, especially in complex flue gases.
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
Nanoscale
·
2024
·
IF 5.8
Jie Zhang,Kongjun Zhu,Zhihan Kong,Dingwei Ji,Jun Guo,Zheng Zhang,Jing Wang,Kang Yan,Jinsong Liu
An all-vanadium-based lithium–ion full battery is successfully assembled with the hierarchical micro–nano yolk–shell structure V2O5 and V2O3 as cathode and anode, which are obtained through a facile solvothermal method with heat treatment under different atmospheres. When used as the cathode of lithium–ion battery, the hierarchical micro–nano yolk–shell V2O5 demonstrated higher capacities than bulk V2O5, commercial LiFePO4, and LiNi0.8Co0.1Mn0.1O2 cathodes at various current densities. The all-vanadium-based lithium–ion full battery shows good cycle performance at 0.1C and stable charge/discharge abilities at large current densities. The electrochemical performance of the full battery results from the low impedance and pseudocapacitance-dominated lithium storage mechanism derived from micro–nano yolk–shell structure.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Waste Disposal & Sustainable Energy
·
2023
·
IF 0
Wang Ling,Tang Minghui,Li Hongxian,Ding Jiamin,Qiu Juan,Lu Shengyong
Polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) have attracted widespread concern due to their high toxicity, and their difficult manipulation in laboratories has made the research process tough. Thus, in our work, furan is selected as the model compound owing to the same structure of a central oxygenate ring. Although catalytic oxidation is regarded as an effective and applicable method for the abatement of PCDD/Fs, the synthesis of low-temperature catalysts is still a challenging problem in practical applications. Considering this situation, we prepared a novel V 2 O 5 /TiO 2 catalyst modified with N-doped hierarchical porous carbon (NHPC) via a wet impregnation method. The V/T-1%NHPC catalyst could achieve expectant low-temperature performances with 50% furan conversion at 150 °C and a complete conversion at 200 °C, which decreased 23 °C and 40 °C compared to the V/T catalyst respectively. Moreover, the addition of NHPC presented lifting chemical stability during long-time test. The addition of NHPC in V/T catalysts decreased the formation of crystalline V 2 O 5 and increased the percentages of V 5+ and O lat , which improved the utilization of vanadium ions and the catalytic activity. Simultaneously, the higher binding energy shift of O lat implied more reaction possibility with other oxidise reactants. Importantly, this work proved the lifting catalytic activity by the interaction between catalysts and NHPC, and proposed the promoting effects of the N element. The results showed that the content of the pyridinic N and graphitic N in NHPC changed after combining with V/T catalyst, which played crucial roles in the excellent catalytic performance. Overall, this work provides comprehensive research of the V/T-1%NHPC catalyst toward furan oxidation at low temperature and explain the effects of N-doped biomass carbon in catalytic activity clearly, which gave a new thought to design low-temperature catalysts in PCDD/Fs degradation. Besides, the internal functional mechanisms of N species are worth further exploration in future studies. Graphical abstract
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
DOI
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 8
·2008033
·
IF 16.836
Ying Liu,Yue Jiang,Zhe Hu,Jian Peng,Weihong Lai,Dianlun Wu,Shouwei Zuo,Jing Zhang,Bin Chen,Ziwen Dai,Yingguo Yang,Yang Huang,Wei Zhang,Wei Zhao,Wang Zhang,Lei Wang,Shulei Chou
Vanadium-based materials are fascinating potential cathodes for high energy density Zn-ion batteries (ZIBs), due to their high capacity arising from multi-electron redox chemistry. Most vanadium-based materials suffer from poor rate capability, however, owing to their low conductivity and large dimension. Here, we propose the application of V 2 C MXene (V 2 CT x ), a conductive 2D nanomaterial, for achieving high energy density ZIBs with superior rate capability. Through an initial charging activation, the valence of surface vanadium in V 2 CT x cathode is raised significantly from V 2+ /V 3+ to V 4+ /V 5+ , forming a nanoscale vanadium oxide (VO x ) coating that effectively undergoes multi-electron reactions, whereas the inner V-C-V 2D multi-layers of V 2 CT x are intentionally preserved, providing abundant nanochannels with intrinsic high conductivity. Owing to the synergistic effects between the outer high-valence VO x and inner conductive V-C-V, the activated V 2 CT x presents an ultrahigh rate performance, reaching 358 mAh g −1 at 30 A g −1 , together with remarkable energy and power density (318 Wh kg −1 /22.5 kW kg −1 ). The structural advantages of activated V 2 CT x are maintained after 2000 cycles, offering excellent stability with nearly 100% Coulombic efficiency. This work provides key insights into the design of high-performance cathode materials for advanced ZIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Xiaohong Chen,Xuezhen Zhai,Yongqi Wu,Xuzhe Wang,Lamei Zhang,Cui Shang,Huawei Zhang,Chengzhou Zhao,Jimin Shang,Dewei Liu
Vanadium-based oxides have gained significant attention as promising cathode materials for aqueous zinc-ion batteries, owing to their high theoretical capacities, the ability to undergo multi-electron transfer, and varied crystal structures. Despite these advantages, challenges related to structural instability and poor electrical conductivity remain significant barriers to their practical application. In this study, Cr-doped VO 2 (B) nanorods were prepared using a hydrothermal treatment process as a promising candidate for aqueous zinc-ion battery cathodes. The multivalent nature of vanadium promotes a variety of redox reactions, resulting in high specific capacities. Chromium ion doping increases oxygen vacancy defects and provides efficient channels for electron transfer. The nanorod morphology offers an increased specific surface area, thereby promoting a higher density of active sites. Positron annihilation lifetime spectroscopy indicates that the generated defects exist in the form of single vacancies. Thanks to the unique tunnel structure and micro-morphology advantages, the CrVO cathode exhibits rapid electron transfer and superior reaction kinetics. Electrochemical performance is optimized at a chromium ion doping concentration of 6 at.%, achieving a high specific capacity of 312.8 mAh g −1 at 0.1 A g −1 and retaining 188.3 mAh g −1 at 5 A g −1 after 2000 cycles, with a remarkable capacity retention of 90.39 %, indicating exceptional long-term cycling stability. This work optimizes the electrochemical performance by introducing different concentrations of chromium ions into the monoclinic VO 2 , thereby altering the Cr 3+ /Cr 6+ and V 4+ /V 5+ ratio, providing a feasible approach for developing high-performance vanadium-based aqueous zinc-ion battery cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Fujie Liu,Tianqi Huang,Mengyue Chen,Jing He,Hongping Li,Chao Wang,Huaming Li,Ming Zhang
Due to the increased concern on the environmental issues, the desulfurization process in fuel is of great importance in the recent decades. Herein, a series of decavanadate-based poly (ionic liquids) with varied substituents were successfully prepared by a facile ion exchange method, which were employed in aerobic oxidative desulfurization of aromatic sulfides. The prepared samples can achieve deep desulfurization on different aromatic sulfides under optimal reaction conditions. Additionally, the experimental results indicated that the long carbon chains in the imidazole ring could hinder the ion exchange process between decavanadate and PILs due to steric hindrance effect, resulting in the poor desulfurization activity. Finally, a possible reaction mechanism was proposed according to the results of XPS, ESR and GC–MS analysis.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Applied Ceramic Technology
·
2023
·Vol. 21
·期 1
·319-326
·
IF 2.1
Jiajia Song,Lingjiang Kou,Yong Wang,Taotao Ai,Wenhu Li,Koji Kajiyoshi,Panya Wattanapaphawong,Yi Li
Energy density, power density, as well as the cost of aqueous zinc-ion batteries (AZIBs), are largely determined by the cathode material. Among the various cathodic candidates, vanadium-based materials with various oxidation states of vanadium cations and open frameworks have emerged as highly promising options. In this work, a heterogeneous with hydrangea-like (NH 4 ) 2 V 4 O 9 /V 5 O 12 ·6H 2 O as cathode materials for AZIBs. The hydrogen bonds formed by NH 4 + of (NH 4 ) 2 V 4 O 9 , in conjunction with the lattice water in V 5 O 12 ·6H 2 O, sufficiently strengthen the cohesion of the layered structure and expand the interlayer space. As a result, accelerating the diffusion of Zn 2+ ultimately leads to an enhanced overall discharge capacity. Remarkably, the hydrangea-like (NH 4 ) 2 V 4 O 9 /V 5 O 12 ·6H 2 O electrode at a current density of 100 mA g −1 shows a high reversible capacity of 209 mAh g −1 after 150 cycles and higher rate capability (172 mAh g −1 at 500 mA g −1 ). The outstanding electrochemical performance can be attributed to the unique structure of the cathode material and accelerated diffusion coefficient of Zn 2+ .
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）