Lubricants
·
2024
·Vol. 12
·期 5
·163
·
IF 3.1
Yunqi Fang,Yang Sun,Fengqin Shang,Jing Zhang,Jiayu Yao,Zihan Yan,Hangyan Shen
Van der Waals heterostructures with incommensurate contact interfaces show excellent tribological performance, which provides solutions for the development of new solid lubricants. In this paper, a facile electrostatic layer-by-layer self-assembly (LBL) technique was proposed to prepare multi-layer van der Waals heterostructures tungsten disulfide/hexagonal boron nitride (vdWH WS2/h-BN). The h-BN and WS2were modified with poly (diallyldimethylammonium chloride) (PDDA) and sodium dodecyl benzene sulfonate (SDBS) to obtain the positively charged PDDA@h-BN and the negatively charged SDBS@WS2, respectively. When the mass ratio of PDDA to h-BN and SDBS to WS2were both 1:1 and the pH was 3, the zeta potential of PDDA@h-BN and SDBS@WS2were 60.0 mV and −50.1 mV, respectively. Under the electrostatic interaction, the PDDA@h-BN and SDBS@WS2attracted each other and stacked alternately along the (002) crystal plane forming the multi-layer (four-layer) vdWH WS2/h-BN. The addition of the multi-layer vdWH WS2/h-BN (1.0 wt%) to the base oil resulted in a significant reduction of 33.8% in the friction coefficient (0.104) and 16.8% in the wear rate (4.43 × 10−5mm3/(N·m)). The excellent tribological property of the multi-layer vdWH WS2/h-BN arose from the lattice mismatch (26.0%), a 15-fold higher interlayer slip possibility, and the formation of transfer film at the contact interface. This study provided an easily accessible method for the multi-layer vdWH with excellent tribological properties.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Shiwen Wang,Chuanzhen Ma,Junwei Ding,Kang Zhao,Heng Wang,Hewei Luo,Shide Wu,Shaoming Fang
VO 2 (B) has attracted tremendous attention as a cathode for aqueous zinc-ion batteries (AZIBs), but its low intrinsic electronic conductivity and uncontrolled vanadium dissolution hinder further practical applications. Herein, Zn 0.03 VO 2 , with guest zinc ions preinserted into the tunnel sites, is demonstrated to enhance the conductivity and cyclability of VO 2 (B). The tailored structure, featuring a modulated electronic configuration, offers enlarged ion diffusion tunnels, improved electronic conductivity, and enhanced electrochemical activity, thereby facilitating the reversible de-intercalation of Zn 2+ /H + ions, as confirmed by both experimental results and theoretical calculations. Notably, vanadium dissolution is significantly suppressed due to the chemical pre-insertion of guest zinc, which weakens the interaction between Zn 2+ and host lattice, as well as the homologous ion effect. As a result, Zn 0.03 VO 2 cathode delivers a high capacity of 358 mAh g −1 , particularly at low current density of 0.1 A g −1 , with 85% capacity retention after 300 cycles, excellent rate capability of 175 mAh g −1 at 5 A g −1 , and long cycling stability over 2000 cycles at 20 A g −1 . Moreover, a pseudocapacitive-dominated Zn 2+ /H + co-insertion mechanism is conclusively identified through electrochemical and spectroscopic analyses. This work provides valuable insights into ion-preinserted structural modulation of vanadium oxides for the development of high-performance AZIBs.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Zhiwei Zou,Hongxiang Zhang,Xuefeng Pan,Hui Shen,Jianying Yu,Tengfei Guo,Yonghao Wang
Electrocatalytic reduction of nitrate (NO 3 - ) to ammonium (NH 4 + ) is an environment friendly approach for treating nitrogen-containing wastewater. Consequently, electrocatalysts capable of effectively and selectively reducing NO 3 - to NH 4 + receives growing attention. However, Cu-based catalysts demonstrate limited efficiency and the drawback of generating toxic NO 2 - though it is prevalent in the field of electrocatalytic reduction of NO 3 - (NO 3 RR). In this work, a CuNi alloy was synthesized on a Co foil through electrodeposition (marked as CuNi@Co) and its electrocatalytic performance for NO 3 RR was evaluated. XRD, EDS mapping and XPS characterization indicate CuNi exists with alloy state. Electrocatalytic experiments demonstrate that CuNi@Co exhibits an exceptional FE NH3 of 99.12% at -0.64 V (vs. RHE). Importantly, no detrimental NO 2 - generated during NO 3 RR process because the reduction rate from NO 2 - to NH 4 + is faster than that from NO 3 - to NO 2 - . Mechanistic analysis suggests that Cu serves as a ‘reservoir’ to provide electrons to facilitate the reduction of NO 3 - to NO 2 - during NO 3 RR process and the synergistic effect of Ni and Cu promotes more active hydrogen (H*) to participate the reduction process of NO 2 - to NH 4 + not H 2 generation, ultimately improving FE NH3 . This work elucidates the role of electrons and H* in electrocatalytic nitrate reduction to ammonium for CuNi alloy, providing new insights into the reduction process of NO 3 RR for Cu-based materials.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Ling Ding,Lou Gao,Di Pan,Ke Du,Jiayu Yu,Wanyi Li,Yahong Zhang,Yi Tang
The utilization of racemic lactic acid (rac-LA) produced via chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (meso-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of meso-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L2A) in a one-step catalytic conversion of rac-LA to LD. Experimental results from various LA solutions with different L2A content indicate that the L2A content is critical for maximizing the selectivity of racemic lactide (D/L-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L2A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease meso-LD formation, and a LD yield of 60% with a D/L-LD/meso-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of D/L-LD and meso-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from rac-LA derived from chemical conversion.
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ACS Catalysis
·
2024
·
IF 11.3
Zaixiang Xu,Fengcang Zhou,Hanchi Chen,Jianguo Wang
The regeneration of NAD(P)H and its analogues is crucial for biocatalytic processes. However, despite the efficiency of enzymatic catalysis in regenerating NAD(P)H, the sustainability of enzymes is often compromised, particularly under extreme catalytic conditions. Moreover, artificial cofactors may present advantages in certain reactions due to their stability and versatility, yet the substrate specificity of enzymes poses significant challenges to their regeneration through the enzymatic method. Therefore, it is imperative to develop a highly stable regeneration method that can be adapted to both natural and artificial cofactors. In this work, employing potassium-ion-doped carbon nitride (ionCN-0.2) as a catalyst not only achieves high-efficiency photocatalytic regeneration of NAD(P)H, comparable to that of glucose dehydrogenase (GDH), but also a remarkable ability to regenerate nicotinamide analogues. This enhanced performance stems from the tunable negative ζ-potential, which effectively adsorbs the positively charged [Cp*Rh(bpy)H2O]2+ mediator, resulting in enhanced regeneration kinetics of the nicotinamide moiety. The catalyst demonstrates superior performance compared to the reported systems; the optimal regeneration rate reaches 0.55 mmol L–1 gcat–1 min–1 and approaches enzymatic regeneration efficiency. Expanding the reaction conditions to a wider temperature and pH range also confirms the effectiveness and sufficient stability of this photocatalytic system, offering a promising strategy for stable cofactor regeneration in biocatalytic processes.
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ChemistrySelect
·
2025
·Vol. 10
·期 7
·e202405464
·
IF 2
Kun Jia,Peng Jia
Graphical The asymmetric activation of anhydrous methanol molecules is realized by exogenous protons, the position and protonation position of asymmetric activation are determined, and the C─H bonding energy and reaction activation energy of some methanol molecules are reduced, and the asymmetric regulation of the non-oxidation dehydrogenation reaction process of anhydrous methanol molecules was realized. The activation of C─H bonds under mild conditions is a crucial step in the conversion of organic molecules. However, the simultaneous activation of C─H bonds in methanol can result in excessive oxidation, thereby diminishing the selectivity for formaldehyde production. We achieved selective activation of the C─H bonds in methanol under mild conditions by adjusting the proton concentration in an anhydrous methanol solution, which significantly enhanced the dehydrogenation rate of methanol. Additionally, we constructed related molecular models to identify the sites of asymmetric oxidation, providing new insights for further studies on C─H bond activation.
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RENEWABLE ENERGY
·
2024
·
IF 9
Huajing Zhou,Tiancheng Li,Fawen Zhang,Faze Chen,Zilian Liu,Rongrong Miao,Qingqing Guan,Lingxiang Zhao,Liang He
Intrinsic point defects in metal core-shell materials can regulate electron redistribution, thereby reducing catalytic energy barriers and enhancing their ORR activity. However, their specific contributions to electron transfer and mass transport pathways remain unclear. In this study, defect-rich hollow O Co @Co 3 O 4 nanoparticles were successfully synthesized using ZIF-67(Co) as a sacrificial template through controlled annealing and internal electric field substitution reactions. High-resolution electron microscopy analysis and density functional theory (DFT) calculations co-revealed the growth mechanism of Co and O vacancies, as well as antisite defects. The formation of oxygen vacancies significantly lowered the energy barrier for Co vacancy formation, playing a crucial bridging role in the development of antisite defects. The electric field polarization induced by Co-O atomic displacement resulted in asymmetric charge distribution, optimizing the adsorption of active hydrogen (H*) and oxygen atoms and facilitating the generation and release of reactive oxygen species (ROS). Electrocatalytic experiments demonstrated that under the combined action of singlet oxygen ( 1 O 2 ) and H*, bisphenol A (BPA) can be efficiently degraded. This study successfully bridges the knowledge gap between atomic defects and advanced electrocatalysis, providing a new perspective and insight for the in-depth analysis of the structure-performance relationship of electrocatalyst materials in the future.
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Joule
·
2020
·
IF 29.155
Anyi Mei,Yusong Sheng,Yue Ming,Yue Hu,Yaoguang Rong,Weihua Zhang,Shulin Luo,Guangren Na,Chengbo Tian,Xiaomeng Hou,Yuli Xiong,Zhihui Zhang,Shuang Liu,Satoshi Uchida,Tae-Woong Kim,Yongbo Yuan,Lijun Zhang,Yinhua Zhou,Hongwei Han
Summary The stability of perovskite solar cells (PSCs) has been considered as the largest obstacle to their commercialization. Herein, we observed that the main failure mechanism for MAPbI 3 perovskite is the escape of methylammonium (MA) iodide at the grain boundaries in an open space or the reconstruction of crystal in a confined small space, as well as the irreversible long-distance ionic migration under the multiple actions of light, heat, and electrical bias. Strengthened with bifunctional organic molecular of 5-ammoniumvaleric acid (5-AVA) iodide at the grain boundaries, the MAPbI 3 crystal was localized in the nanoscale, and thus, the decomposition or reconstruction was inhibited and the ionic migration became reversible. As a result, we propose a reliable approach to make PSCs meet stability standards of IEC61215:2016 qualification tests. A printable PSC filled with (5-AVA) X MA 1-X PbI 3 has been working for more than 9,000 h at a maximum power point of 55°C ± 5°C without obvious decay.
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ACS Catalysis
·
2025
·
IF 13.1
Yu-Yang Liu,Shan Xu,Xiao-Xin Li,Run-Han Li,Xin-Ting Cai,Hui-Zhen Zhong,Jiang Liu,Qing Huang,Lei Zhang,Shun-Li Li,Ya-Qian Lan
Developing strategies and photocatalysts for C(sp3)-H bond functionalization under simple and mild conditions is important but challenging. Here, we report two redox heterocluster-based frameworks, named Ni5-PW12 and Ni5-V16, in which the terminal oxygen atoms of polyoxometalates are directly coordinated to metal atoms in metal–organic clusters. Due to the coexisting strong oxidation and reduction capacities, both of these photocatalysts achieve photocatalytic C(sp3)-H bond oxidative imination through combining oxidation of methyl aromatics and reduction of nitro aromatics reactions. The experimental and theoretical results reveal that benefiting from the short distance between the clusters, the rapid charge transfer and mass transfer processes would enhance the photocatalytic reactivity and inhibit side reactions. More importantly, all of the photocatalytic reactions are carried out in mild conditions at room temperature without any additional solvents, photosensitizers, oxidizing or reducing agents, or cocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Tian Huang,Jing Zhao,Haijun Li,Wei Zhou,Jintao Wang,Jianliang Shen,Jicai Chen,Xiangwen Liao
Infections caused by methicillin-resistant Staphylococcus aureus ( MRSA ) are a significant public health challenge, necessitating the development of innovative antibacterial strategies. Nanomaterials are recognized for their ability to serve as photothermal conversion agents, transforming light energy into heat for antibacterial applications. These materials act as biological enzymes capable of generating reactive oxygen species (ROS), leveraging their catalytic activity to combat infections. While they show considerable promise, enhancing their ROS-generating efficiency and overall catalytic performance remains a critical challenge. In this work, a high catalytic bimetallic nanoplatform was developed, building on “large electronegativity difference induction/etch-assisted/diffusion termination” mechanism to improve antibacterial efficacy. The synthesized nanoparticles were found to exhibit exceptional photothermal conversion efficiency and surface defects, enabling efficient bacterial eradication. Both in vitro and in vivo experiments demonstrated that H-Pt 3 Sn nanoparticles effectively eliminated MRSA while significantly inhibiting and disrupting biofilms formed by the pathogen. The nanoparticles also facilitated tissue repair by modulating macrophage-related molecular markers. In conclusion, this study presents a promising photothermal synergistic nanosystem with high catalytic functionality for advanced anti-infective applications.
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JOURNAL OF MASS SPECTROMETRY
·
2015
·Vol. 50
·期 1
·212-219
·
IF 2.379
Huixin Wang,Bing Wang,Zhonglin Wei,Hao Zhang,Xinhua Guo
A good understanding of gas-phase fragmentation chemistry of peptides is important for accurate protein identification. Additional product ions obtained by sodiated peptides can provide useful sequence information supplementary to protonated peptides and improve protein identification. In this work, we first demonstrate that the sodiated a 3 ions are abundant in the tandem mass spectra of sodium-cationized peptides although observations of a 3 ions have rarely been reported in protonated peptides. Quantum chemical calculations combined with tandem mass spectrometry are used to investigate this phenomenon by using a model tetrapeptide GGAG. Our results reveal that the most stable [a 3 + Na − H] + ion is present as a bidentate linear structure in which the sodium cation coordinates to the two backbone carbonyl oxygen atoms. Due to structural inflexibility, further fragmentation of the [a 3 + Na − H] + ion needs to overcome several relatively high energetic barriers to form [b 2 + Na − H] + ion with a diketopiperazine structure. As a result, low abundance of [b 2 + Na − H] + ion is detected at relatively high collision energy. In addition, our computational data also indicate that the common oxazolone pathway to generate [b 2 + Na − H] + from the [a 3 + Na − H] + ion is unlikely. The present work provides a mechanistic insight into how a sodium ion affects the fragmentation behaviors of peptides. Copyright © 2015 John Wiley & Sons, Ltd.
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PubMed
高影响因子
ACS Nano
·
2023
·
IF 17.1
Changhao Zhu,Xuye He,Yun Shi,Zhenkang Wang,Baojiu Hao,Wanhao Chen,Hao Yang,Lifang Zhang,Haoqing Ji,Jie Liu,Chenglin Yan,Jinqiu Zhou,Tao Qian
Despite the numerous advantages of aqueous Zn batteries, their practical application under cryogenic conditions is hindered by the freezing of the electrolyte because the abundance of hydrogen bonds (H-bonds) between H2O molecules drives the aqueous system to transform to an orderly frozen structure. Here, a design of H-bond interactions based on the guiding ideology of “strong replaces weak” is proposed. The strong H-bonds formed between introduced eutectic components and water molecules break down the weak H-bonds in the original water molecule network, which contributes to an ultralow freezing point and a high ionic conductivity of 1.7 mS cm–1 at −40 °C. Based on multiperspective theoretical simulations and tailor-made in situ cooling Raman characterizations, it has been demonstrated that substituting weak H-bonds with strong H-bonds facilitates the structural reshaping of Zn2+ solvation and remodeling of the H-bond network in the electrolyte. Endowed with this advantage, reversible and stable Zn plating/stripping behaviors could be realized at −40 °C, and the full cells display a high discharge capacity (200 mA h g–1) at −40 °C with ∼75% capacity retention after 1000 cycles. This study will expand the design philosophy of antifreezing aqueous electrolytes and provide a perspective to promote the adoption of Zn metal batteries for cryogenic environment large-scale energy storage.
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