查找使用阿拉丁产品的科研文献

Two-dimensional sandwich-like heterostructures of amorphous VOx/MXene as freestanding cathode materials with superior electrochemical performance for aqueous zinc-ion batteries

Ni Wentao,Yang Hengyu,Liu Xiong,Liang Yongle,Wu Banghui,Zhang Huaijun,Xu Guobao,Wei Xiaolin,Yang Liwen

Although vanadium-based compounds are considered to be reliable zinc storage materials due to their high theoretical specific capacity, notorious poor conductivity and unstable structure hamper their practical applications. Herein, novel two-dimensional (2D) sandwich-like heterostructures of amorphous vanadium dioxide uniformly grown on two sides of ultrathin MXene nanosheets (A-VO x /M heterostructures) are constructed by ion adsorption method and following low-temperature annealing, which can be readily incorporated into carbon nanotube (CNT) network to obtain freestanding cathodes for aqueous zinc-ion batteries. The combination of 2D heterostructure, amorphous framework and conductive substrate endows A-VO x /M heterostructures with short ion diffusion pathway, high chemical stability, extra active sites and superior electrical conductivity. The freestanding A-VO x /M heterostructured cathodes for aqueous zinc-ion batteries exhibit a remarkable discharge capacity of 362 mAh g −1 at 0.2 A g −1 and high-rate capability of 202 mAh g −1 at 15 A g −1 as well as admirable cycling stability with a capacity decay of only 0.0043% per cycle over 3000 cycles. Besides, due to the outstanding conductivity and stability of freestanding A-VO x /M heterostructured cathodes, soft-package batteries are assembled with steady electrochemical performance, suggesting brilliant future in the field of energy storage.

Accelerated vanadium (IV)/(V) redox cycle and hydroxyl radical generation by hydroxylamine in peroxymonosulfate activation: from synthetic vanadium oxides to natural minerals

Ge Li,Yujie Cheng,Yiqun Chen,Zizheng Liu,Jun Ma,Pengchao Xie

Vanadium-based catalysts face challenges in advanced oxidation processes (AOPs) due to the instability of expensive V(IV) and the weak catalytic activity of V(V). This study, leveraging the strong reducing ability of hydroxylamine (HA), developed the HA/V 2 O 5 /peroxymonosulfate (PMS) system. Under the condition of 100 μM PMS and 0.2 g/L V 2 O 5 , the addition of 200 μM HA accelerated the vanadium (IV)/(V) redox cycle, thereby increasing the degradation efficiency of sulfamethoxazole (SMX) from 18.3 % to 98.3 %. HO • was identified as the dominant reactive oxygen species (ROS) by quenching and probe experiments in the system, which was capable of non-selectively and efficiently degrading a wide range of micro-pollutants. Additionally, the degradation pathways and intermediate products of SMX and HA were investigated. HA was primarily converted into environmental friendly N 2 and NO 3 − , and significant reductions in the bioaccumulation factor, developmental toxicity, and mutagenicity of most SMX intermediate products were achieved. Finally, a comparative study evaluated the activation efficiency of natural vanadium‑titanium magnetite (VTM) and synthetic vanadium oxides in practical application scenarios, highlighting the high efficiency, stability and low cost of VTM compared to other reported catalysts.

The Role of V-Species and O-Species on Controlled-Hydrogen-Reduction VOx Surfaces in Cyclohexane Oxidation

Yingwei Li,Shengxin Chen,Ying Jin,Xinxin Li,Ruirui Zhang,Ruixia Liu

Graphical A simple and controllable defect construction method for vanadium-oxygen catalysts through hydrogen reduction with TCD detector were used to control the reduction state of CHR-VOx which determines the V-Species and O-Species. Furthermore, the structure-performance relationship and the catalytic pathway were assumed, multi-liganded-oxygen and V 4+ species are the key parameters. A series of controlled-hydrogen-reduction VO x (CHR-VO x ) were prepared after our controllable hydrogen treatment, and CHR-VO x were controlled to be reduced to the states dominated by V 5+ and V 4+ species, subsequently the catalytic roles of V-species and O-species for cyclohexane (CHA) oxidation were explored. As expected, the surface properties of CHR-VO x have occurred remarkable change resulting in a significantly improvement on catalytic performance determined by V-species and O-species. The reduction behavior of the properties was recognized by XPS and Raman. Generally, the moderate-reduced CHR-VO x which possessed most 78.7 % multi-liganded-oxygen ( L O) performed the best conversion for CHA (11.8 %), and the over-reduced CHR-VO x with a large content of V 4+ species (33 %) performed a best selectivity for adipic acid (44.3 %). In this case, L O sites were regarded as the active site to accelerate the activation of CHA, while V 4+ species were regarded as the oxygen vacancies (OVs) through V 4+ −OV to contribute to the further oxidation to adipic acid.

Reverse Dual-Ion Battery by Coupling Adsorption and Conversion Mechanism

Yong Li,Jian Zhang,Qingyan Yuan,Yunjia Wu,Jingbin Han

As one kind of promising energy storage device, dual-ion batteries (DIBs) have attracted extensive attention because of their high voltage, environmental friendliness, and low cost. However, they generally suffer from low power density resulting from sluggish kinetic of electrolyte anion intercalation. In this work, a new strategy to break through the trade-off of power density and energy density in DIBs is proposed. A vanadium-doped anatase is synthesized by the hydrothermal method and used as the cathode of DIB (employing Li as the anode). During the charging/discharging process, the organic cations in the electrolyte are reversibly adsorbed–desorbed at the cathode; while a conversion reaction of Li/LiCl occurs at the anode. The effective integration of cation adsorption and conversion reaction mechanism results in a large power density of 1532 W kg −1 along with a high energy density of 214 Wh kg −1 at 1 A g −1 . This design concept is universal and has been successfully transplanted to cation/Br − DIB. Therefore, this work provides a novel approach to optimize the energy/power density of DIBs, which is highly desired in constructing high-performance energy storage devices.

Kaolin supported heteropoly acid catalysts for methacrolein oxidation: Insights into the carrier acidity effect on active components

Qianwen Zhu,Jing Zhu,Yang Li,Zhaobang Zhang,Baohe Wang,Jing Ma

The application of heteropoly acid catalyst in methacrolein (MAL) oxidation reaction is limited for its poor thermal stability and few active centers. Here, the supported catalyst of P-Mo-V heteropoly acid (CsNH 4 KPMoV) active components supported on kaolin were prepared, and were characterized by FT-IR, TG/DTA, XRD, N 2 -adsorption and desorption, NH 3 -TPD, TPO-MS and XPS. The results show that kaolin was weak acidity and the negative charge on the surface of kaolin promoted the reduction of V 5+ species to V 4+ (VO 2+ ) active species. There was a strong electron interaction between kaolin and HPVA, and chemical adsorption occurred by DFT calculations. Under optimal conditions, higher MAL conversion (81.8%) and Methacrylic acid (MAA) selectivity (88.2%) were obtained by 50CsNH 4 KPMoV/kaolin catalyst. The Keggin structure was maintained and the acid strength and acidity did not decrease after the catalyst was used continuously for 100 h. There was no carbon deposition in the reaction process.

Vanadium trioxide mediated peroxymonosulfate for fast metronidazole oxidation: Stepwise oxidation of vanadium for donating electrons

Jiao Shen,Feng Cheng,Yichi Chen,Zeyu Li,Yang Liu,Yue Yuan,Peng Zhou,Wen Liu,Bo Lai,Yongli Zhang

In this study, vanadium trioxide (V 2 O 3 ) was adopted to activate PMS via a Fenton-like reaction to degrade metronidazole (MNZ). The V 2 O 3 -PMS system can almost completely degrade MNZ at 30 min with 42.4% TOC removal. Comparative tests reveal that V 2 O 3 stands out among a variety of heterogeneous catalysts, including metallic oxides and carbon materials. Sulfate radicals (SO 4 •− ) and hydroxyl radicals ( • OH) derived from PMS decomposition are major reactive oxygen species, based on quenching tests, electron spin resonance (ESR) analysis, the steady-state concentrations of radicals ([SO 4 •− ] ss  = 5.1 × 10 -13 M and [ • OH] ss  = 4.0 × 10 -14 M), and kinetics model. The process of stepwise electron transfer from vanadium species to PMS to produce reactive radicals was proved by small-molecule simulation experiments and pickling experiments of vanadium oxides. Possible pathways of MNZ degradation were proposed based on the results of LC-MS and Fukui function, including two stages of the hydroxylation and bond cleavage of nitro and the subsequent ring-opening. This study reveals the high reusability and practicability of the V 2 O 3 -PMS system over a relatively wide pH range, which puts forward a new vision on V 2 O 3 induced Fenton-like reactions and a new reference method for the removal of medical organic contaminants in water.

Repurposing a human acetyl-CoA carboxylase inhibitor firsocostat to treat fungal candidiasis alone and in combination

Tianyu Chen,Jing Yao,Keao Quan,Jingchen Xu,Xudong Hang,Qian Tong,Genyan Liu,Peipei Luo,Liping Zeng,Ganzhu Feng,Hongkai Bi

Polydopamine modified heteropolyacids catalyst for methacrolein oxidation: Organic ammonia functionalized and regulation of morphology

Yang Li,Qianwen Zhu,Yifan Yue,Zhaobang Zhang,Baohe Wang,Jing Zhu,Jing Ma

The oxidation of methacrolein (MAL) to methacrylic acid (MAA) catalyzed by Keggin-type phosphomolybdovanadic acid catalyst belongs to the acid-catalyzed and oxygen-catalyzed co-promoted reactions. It is a challenge to design catalysts with suitable acidity and redox properties. In this paper, a strategy using organic ammonia to modify CsH 3 PMo 11 VO 40 (CsPAV) was proposed. Core-shell polymerization precursors were synthesized by using polydopamine (PDA) microspheres as modifiers and templates, and regularly arranged PDA-CsPAV bowl-shaped catalysts were obtained via one-step calcination. The morphology, structure, thermal stability, acidity and redox properties of PDA-CsPAV catalysts were characterized by XRD, FT-IR, TG-DTA, XPS, SEM, H 2 -TPR and NH 3 -TPD, and the catalytic performance was evaluated by oxidation of MAL to MAA. The rich functional groups on the surface of PDA microspheres combine with H 4 PMo 11 VO 40 (HPAV) through strong coordination bonds to form a catalyst film. The uniform spherical structure of PDA can adjust the dispersion and morphology of CsPAV. NH 4 + was formed and rearranged with heteropoly anions during calcination, which positively regulated the acidity and redox property of the catalyst. The addition of PDA accelerated electron transfer and strengthened the self-reduction process of HPAV. Compared with CsPAV, PDA-CsPAV has more acid sites and oxidation catalytic active centers (VO 2+ ), thus exhibiting better MAL oxidation performance and good thermal stability.

Enhancing Zn-Metal Anode Stability: Key Effects of Electrolyte Additives on Ion-Shield-Like Electrical Double Layer and Stable Solid Electrolyte Interphase

Jianqiang Weng,Wenqi Zhu,Kun Yu,Jing Luo,Meixin Chen,Liuyan Li,Yuhang Zhuang,Kailai Xia,Zhixing Lu,Yajie Hu,Chengkai Yang,Mingmao Wu,Zhigang Zou

Owing to zinc dendrites and parasitic reactions, aqueous Zn-metal batteries often suffer from poor reversibility and cyclability. Electrolyte additives present a promising strategy to improve Zn anode stability. However, the ever-evolving perspectives and mechanisms, paradoxically, complicate battery design, causing a scenario where any electrolyte additive seems to be effective. Herein, it is taken ionic liquid (IL) additives as an example and detailed explored the impact of three typical IL anions, namely OTF − , TFA − , and BF 4 − . It is identified that the primary determinant of electrolyte additives as their electrical double layer (EDL) structures and their subsequent solid-electrolyte interface (SEI) composition. An advantageous EDL structure, akin to an ion-shield, can reduce the absorption of H 2 O molecules, which further enrich the SEI with zincophilic and hydrophobic components, thereby mitigating parasitic reactions and Zn dendrite formation. As a result, the Zn||Zn cell with optimal [EMIM]OTF additives demonstrates an exceptional cycling life under challenging conditions, its cumulative plated capacity surpasses most previously reported results by utilizing different IL additives. This work extends beyond performance enhancements, representing a valuable exploration of key criteria for electrolyte additives is believed. These insights are expected to offer fundamental guidance for future research and electrolyte design.

Graphene acid-enhanced interfacial layers with high Zn2+ ions selectivity and desolvation capability for corrosion-resistant Zn-metal anodes

Kailai Xia,Liuyan Li,Yanbin Qiu,Jianqiang Weng,Shengtao Shen,Meixin Chen,Yuhang Zhuang,Yeye Wen,Chengkai Yang,Zheyuan Liu,Mingmao Wu,Zhigang Zou

Utilizing an interfacial layer to stabilize Zn-metal anodes has been extensively explored, often accompanied by inhibition of Zn dendrites. However, most interfacial layers primarily delay Zn2+ ion transport/transfer, leading to slow Zn deposition due to the ion kinetics hindrance. Basically, this ionic hysteresis effect is inherent to all interfacial layers and will cause unstable Zn deposition over extended cycling periods. Here, we present a simple composite interfacial layer composed of graphene acid (GA) and cellulose nanofibers (CNF). In the CNF/GA layer, a delicate balance between the rapid Zn2+ transport/transfer and uniform Zn deposition is achieved. The presence of GA not only demonstrates excellent ion selectivity and suppresses corrosion reactions, but also promotes Zn2+ transport/transfer, significantly reducing the desolvation energy of Zn2+ ions. Consequently, the symmetric cell with CNF/GA coatings achieves a highly stable cycling life of 2920 h, surpassing previous reports using graphene-based and CNF-based protecting layers. Moreover, the full cell based on the CNF/GA protected anodes exhibits excellent long-term stability and maintains an ultra-stable self-discharge retention of 99% after 24 h of standing. These findings provide valuable insights for the development of protective layers for Zn-metal anode and future grid-scale Zn battery deployment.

Optimizing photoelectrocatalytic Efficiency: Synergistic activation of peroxymonosulfate by CuFeO2/BiVO4 composites for antibiotic removal

Yonglei Xing,Jingyao Duan,Duomin Wang,Xiaoyong Jin,Xin Wang,Rui Yang,Gang Ni

The BiVO 4 photoanode and CuFeO 2 materials were synthesized via electrodeposition and hydrothermal methods, respectively, and the p-n type 2-CBVO (CuFeO 2 /BiVO 4 ) composite photoanode was prepared using a spin-coating technique. The degradation performance of the composite photoanodes was evaluated in a PEC-coupled PMS (peroxymonosulfate) activation system using levofloxacin (LVF) as the target pollutant. The 2-CBVO photoanode achieved a degradation efficiency of 78.8 % for LVF (15 ppm) within 30 min, representing a 45.1 % improvement over the BiVO 4 photoanode. The pseudo-first-order rate constant for the degradation of LVF was determined to be 4.43 × 10 −1 min −1 . Photoelectrochemical analysis confirmed that CuFeO 2 loading and PMS introduction enhanced photogenerated carrier separation, promoting LVF degradation. Radical trapping experiments indicated that h + , OH, SO 4 − and O 2 − were the primary reactive species in the degradation process. Both theoretical calculations and experimental results confirmed that the internal electric field at the composite interface directs from BiVO 4 to CuFeO 2 , facilitating electron transfer from CuFeO 2 to BiVO 4 and onward to the cathode surface via the external circuit. Cyclic stability tests demonstrated that the 2-CBVO composite photoanode retained 90.0 % of its activity after five cycles, indicating excellent stability and significant potential for water treatment applications.

Engineering the conductive network of missing-linker metal-organic framework for improved performance in aqueous zinc-ion batteries

Yuanmei Xu,Xueshi Li,Xiatong Wang,Qijia Weng,Weijun Sun

Aqueous zinc-ion batteries (ZIBs) face critical challenges such as interfacial side reactions, corrosion, and passivation of the zinc anode. In this work, we introduce a novel zinc anode featuring a 3D ordered macroporous (3DOM) architecture based on a missing-linker ZIF-8 framework (Zn@Fc-ZIF-8). This innovative design achieves remarkable stability, maintaining performance for over 4000 h at a current density of 0.25 mA cm −2 in a symmetric cell-over 30 times longer than a bare Zn anode. Additionally, by integrating carbon nanotubes (CNTs) within the 3DOM Fc-ZIF-8 skeleton to create a highly conductive network (3DOM Fc-ZIF-8/CNTs), we extend the anode's lifetime to 1500 h at a high current density of 5 mA cm −2 . The strategic regulation of the ZIF-8 structure using ferrocene formic acid (Fc) and the incorporation of CNTs result in a full cell with the bi-functional Zn@Fc-ZIF-8/CNTs anode, achieving a high specific capacity of 380.5 mAh g −1 and a coulombic efficiency (CE) of 99.8 %. These findings underscore the significant potential of MOF-based anodes in addressing dendrite formation and advancing the practical application of ZIBs.