GREEN CHEMISTRY
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2018
·Vol. 20
·期 11
·2588-2595
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IF 8.586
Da Yang,Huan Liu,Dong-Liang Wang,Zhoujie Luo,Yong Lu,Fei Xia,Ye Liu
A bi-functional ligand (L1) containing a diphosphino fragment and sulfonic acid group (–SO3H) enabled PdCl2(MeCN)2 to efficiently catalyze the tandem bis-alkoxycarbonylation of terminal alkynes to produce aryl-/alkyl-substituted succinate (α,ω-diesters). It was found that the –SO3H incorporated in L1 indispensably assisted the Pd-catalyst in accomplishing this tandem reaction via intramolecular synergic effects. Co-catalysis over the L1-based Pd-catalyst was not due to the physical mixture of Xantphos and MeSO3H. In situ FTIR analysis verified that the formation and stability of Pd–H active species were facilitated by the presence of L1. The formation of stabilized diacylpalladium intermediate (F) was the critical driving force for the second-step methoxycarbonylation. DFT calculation was carried out to optimize the geometric structure of F, which indicated that the developed intramolecular O⋯H hydrogen bonds were an important structural feature to stabilize F. In addition, the L1-based Pd-catalyst could be recycled successfully for at least 3 runs in the ionic liquid [Bmim]NTf2 without obvious activity loss and detectable metal leaching.
研究领域:
有机化学
·
催化化学
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Yue Wei,Gang Li,Jiaxu Liu,Yanhui Yi,Hongchen Guo
The sluggish interfacial mass transfer usually hinders the achievement of high-efficiency catalytic transformation of biomass, especially for solvent-free immiscible reagent systems. Herein, amphiphilic hybrid Ti-containing catalysts in situ incorporated with organic groups (Cn-Ti-HMS) were developed for boosting biphasic solvent-free epoxidation of methyl oleate (MO) with H 2 O 2 . Benefiting from the mutual effect between organic/inorganic precursors, the resulting low-defect catalysts exhibit well-mediated surface hydrophilic/hydrophobic balance and porosity by incorporating alkyl groups. Such mediation effect exhibits two superiorities: i) accelerated adsorption of reactants by amphiphilicity; ii) boosted substrate or product diffusion by porosity property. As such, remarkably promoted catalytic properties were achieved when compared with conventional Ti-HMS. Typically, methyl-functionalized C1–Ti-HMS-50 displays the optimal catalytic performance with a 95% conversion of MO. Further mechanism study recognizes the dominant role of surface wettability and Si–OH defects content in influencing MO conversion and epoxidized MO selectivity.
研究领域:
催化
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材料科学
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化学工程
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环境化学
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JOURNAL OF MATERIALS SCIENCE
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2019
·Vol. 55
·期 9
·4017-4029
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IF 3.442
Wu Ke,Qin Zhaogang,Zhang Xunshuang,Guo Ruichen,Ren Xiaozhen,Pu Xipeng
Researchers have begun to pay close attention to the construction of artificial Z-scheme photocatalysts due to their excellent ability to separate photogenerated electron–hole pairs and prominent redox ability. In this study, Bi-bridged Z-scheme BiOCl/Bi 2 O 3 (BiOCl/Bi–Bi 2 O 3 ) heterojunctions with oxygen vacancies were prepared via a one-step hydrothermal method. The phase structure, morphology, and optical properties of the samples were characterized using XRD, XPS, ESR, FESEM, HRTEM, and UV–Vis DRS. Compared with BiOCl and Bi–Bi 2 O 3 , the prepared BiOCl/Bi–Bi 2 O 3 (25% and 50%) samples exhibited enhanced photocatalytic activity in degrading colorless antibiotics (tetracycline hydrochloride) and colored dyes (RhB) under visible light irradiation. This result indicated improved visible light absorption due to the presence of oxygen vacancies and enhanced separation efficiency of the photogenerated electron–hole pairs and high redox ability due to the construction of the Z-scheme. On the basis of the results of radical-trapping, photoelectron chemical experiments, and PL analysis, a possible photocatalytic mechanism of the Z-scheme BiOCl/Bi–Bi 2 O 3 heterojunctions was proposed.
研究领域:
材料科学
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环境科学
·
化学
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 21
·11445-11453
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IF 11.9
Yumeng Li,Yingmin Jin,Xin Zong,Xuebai Zhang,Guanshu Li,Yueping Xiong
Electrocatalytic carbon dioxide (CO2) reduction reactions (ECO2RRs) to form formate with high faradaic efficiency (FE) and production rate by renewable electricity are ideal to control CO2 concentration in the atmosphere. In this work, we successfully prepared bimetallic BixIny nanofiber (NF) catalysts with interconnected 3D network structure and controllable growth direction of crystal facets via electrospinning and the following electrochemical reduction for the first time, rendering a significantly increased InBi (200) lattice plane proportion in Bi5In5 NFs, which facilitated the improvement of intrinsic catalytic activity and formate selectivity for ECO2RR catalysts, as evidenced by crystalline characterization and DFT calculations. Consequently, the obtained Bi5In5 NFs achieve a maximum FE of 96.8% for formate and the corresponding production rate can reach 4.55 mmol h−1 cm−2, superior to most of the formate producing catalysts. This work provides a novel approach for preparing bimetallic catalyst NFs with high FE and product selectivity; moreover, the favorable productivity brings substantial application potential in industrial production.
研究领域:
材料科学
·
电化学
·
催化
·
环境科学
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高影响因子
Journal of Energy Chemistry
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2022
·
IF 13.599
Jun Yang,Jiahui Xian,Qinglin Liu,Yamei Sun,Guangqin Li
Bismuth (Bi) has indeed inspired great interests in lithium-ion batteries (LIBs) due to the high capacity, but was still limited by the low electrical conductivity and large volume variation. Herein, a composite material based on Bi nanoparticles in situ encapsulated by carbon film (Bi@CF) is prepared successfully through a facile metal–organic framework (MOF)-engaged approach. As anode materials for LIBs, the Bi@CF composites achieved high reversible capacities of 705 and 538 mAh g −1 at 0.2 and 0.5 A g −1 after 200 cycles, and long cycling performance with a stable capacity of 306 mAh g −1 at 1.0 A g −1 even after 900 cycles. In situ X-ray diffraction (XRD) measurements clearly revealed the conversion between Bi and Li 3 Bi during the alloying/dealloying process, confirming the good electrochemical reversibility of Bi@CF for Li-storage. The reaction kinetics of this Bi@CF composite was further studied by galvanostatic intermittent titration technique (GITT). This work may provide an inspiration for the elaborate design and facile preparation of alloy-type anode materials for high-performance rechargeable batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Yuanxiang Zhang,Maosheng Cui,Mengting Yuan,Zhen Mu,Han Wang,Xinchun Zhou,Yang Zhang,Lingxiu Chen,Xiaolan Xue
Magnesium metal batteries (MMBs) are promising candidates for sustainable energy storage, yet their development is severely hindered by the formation of passivation layers on the Mg anode. Conventional artificial interphase layers often suffer from progressive defunctionalization during prolonged cycling. Herein, we propose a chemical-dissolution-equilibrium-driven strategy that continuously supplies Bi3+ species to spontaneously construct an in situ Mg3Bi2/Bi protective layer on the Mg electrode surface. This self-sustaining interphase not only enables continuous interfacial repair but also provides abundant magnesiophilic nucleation sites, thereby facilitating highly efficient Mg plating/stripping. As a result, the Mg||Mg symmetric cell exhibits an ultralong cycling life exceeding 1500 h with an ultralow overpotential of 30 mV at 0.5 mA cm–2 and 0.25 mAh cm–2. Moreover, the preferential reduction of Bi3+ on various current collectors creates favorable nucleation sites for Mg deposition, leading to high Coulombic efficiencies in Mg||Cu, Mg||SS, and Mg||Mo asymmetric cells. Remarkably, the Mg||SS cell achieves a cycling life exceeding 1400 h with an average Coulombic efficiency of ∼99.84% and a low polarization voltage of 90 mV. This work underscores the critical role of a sustained dynamic interphase and establishes a new paradigm for designing nonaqueous, all-inorganic electrolytes for high-performance MMBs.
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Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·346
·
IF 38.5
Chen Jiajie,Huang Jimin,Yang Zhibo,Tang Kai,Wu Chengtie,Ye Huamao,Shi Jianlin,Zhu Yufang
Diabetes aggravates postoperative tumor recurrence and impairs wound healing due to divergent metabolic adaptations to hyperglycemia in tumor versus normal cells. Current therapeutics fail due to the incapabilities in adaptively modulating the metabolic bifurcation across the contradictory pathological contexts. Here, we address this challenge by developing a platinum (Pt) single-atom nanocatalyst (PtSNC) with microenvironments-selective multienzyme-mimicking activities to pioneer a bi-polar bioenergetic intervention strategy. In acidic and reduced nicotinamide adenine dinucleotide (NADH)-overexpressed tumor niches, it exhibits NADH oxidase (NOX)-, oxidase-, and peroxidase-like activities, depleting NADH reserves and generating highly reactive Pt = O species to disrupt energy metabolism and induce both apoptosis/ferroptosis. While it shows NOX-, catalase-, and superoxide dismutase-like activities in neutral diabetic wounds, rectifying hyperglycemia-induced cellular NAD + /NADH abnormity and bioenergetic disorder to revitalize the cells and tissues, with promoting angiogenesis and mitigating local inflammation to accelerate regeneration. Murine diabetic melanoma resection models demonstrate its extensive capacity in effectively eradicating residual tumor tissues and suppressing the recurrence, and promoting diabetic wound healing concurrently without systemic toxicity, making PtSNC a safe and potent nanotherapeutic for diabetic tumor postoperative therapy. This study holds promise for the application of single-atom catalytic medicines in precision therapy for intractable diseases featuring pathological metabolic bifurcation. The alternative text for this image may have been generated using AI.
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PubMed
高影响因子
PROGRESS IN ORGANIC COATINGS
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2026
·
IF 7.9
Yan Zhang,Ziqing Jiang,Jiayu Lu,Bibo Wang,Jinling Liu,Yanyan Wang,Zhien Zheng,Dongming Qi,Wei Wang
Conventional electromagnetic interference (EMI) shielding materials predominantly reflect waves, causing secondary pollution, while achieving absorption-dominated shielding without complex structures or magnetic components remains a significant challenge. Inspired by the scrub sponge architecture, this study develops a CNTs/MF-PA foam-film composites with modular bi-conductive networks for tunable absorption-dominated EMI shielding, where the porous foam serves as a regulatory component that modulates the electromagnetic response of the underlying organic coating. The asymmetric design, combining a carbon nanotube-loaded melamine foam (CNTs/MF) with a replaceable silver nanowire-based organic coating (PA), achieves 76.89 dB shielding effectiveness (SE) and 0.94 absorption coefficient (A) without magnetic components. Notably, by interchanging the bottom coating with varying EMI SE (20–80 dB), the overall shielding performance can be precisely tuned while maintaining an ultra-high A above 0.93, demonstrating universal foam regulation of different coatings for customizable shielding. The superior performance stems from synergistic effects where the foam layer ensures excellent impedance matching, promotes multiple scattering, and induces phase cancellation through extended propagation paths, while the organic coating provides robust shielding. This work offers a groundbreaking strategy for developing functional organic coating materials with tailored electromagnetic performance, holding immense promise for applications in flexible electronics and advanced aerospace systems.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2026
·
IF 8.7
Yuxuan Guo,Yueyuan Xu,Yueqi Zhou,Canming Hu,Chengli Ding,Abulikemu Abulizi
The use of photogenerated carriers to regulate interfacial photo-redox reactions and improve the efficiency of photocatalytic applications has become a hot topic in photocatalyst research. We proposed a novel strategy, which enables efficient charge separation by uniformly deposition CuS/Bi₂S₃ nanoparticles on three-dimensional porous cellulose-derived carbon aerogel (CA), and utilizes highly active holes excited by ultraviolet-visible light to drive surface reactions, demonstrating excellent performance in the photo-oxidative degradation of methylene blue (MB) organic pollutants. The samples were characterized and structurally tested using techniques such as X-ray fluorescence spectroscopy, X-ray diffraction analysis, scanning electron microscopy, and a BET specific surface area analyzer. Under visible light irradiation, the composite material demonstrated remarkable degradation efficiency for methylene blue, achieving 98.98% removal within 80 min while maintaining over 87.48% of its initial activity after five consecutive reaction cycles. The enhanced photocatalytic performance is attributed to the fact that the carbon aerogel matrix provides a 3D framework with high surface area to effectively disperse catalyst nanoparticles and organic dye molecules near the active site, its conductive network facilitates efficient electron transport, and the porous structure can optimally separate photogenerated electron-hole pairs by enhancing light absorption through internal scattering mechanisms. We identified that superoxide anions (·O₂ − ) and hydroxyl radicals (·OH) act as the primary active species in the degradation process through radical trapping experiments. This study not only presents a high-performance, environmentally friendly catalyst for wastewater treatment but also offers valuable design principles for developing biomass carbon-based photocatalytic systems with S-scheme heterojunctions.
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PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2026
·
IF 6.2
Xueqiong Lei,Fan Zhang,Xin Wang,Xiaoyue Ma,Xinhui Li,Chao Wang,Tailong Che,Changlong Li,Zhan Jie Wang
Due to their exceptional power density and fast charge–discharge performance, dielectric ceramic capacitors have emerged as vital components in advanced pulsed power systems. However, concurrently achieving excellent recoverable energy density (Wrec) and high efficiency (η) in lead-free systems remains challenging. Herein, a multi-scale high-entropy design strategy is proposed for (Bi0.5Na0.5)0.94Ba0.06TiO3-based relaxor ferroelectrics. The approach involves sequentially introducing (Sr0.7Bi0.2)TiO3 and (Bi0.5La0.5)(Nb1/3Mg2/3)O3 to construct a high-entropy system that simultaneously regulates material behavior across lattice, microstructural, and electronic structure scales. This coordinated approach induces strong lattice distortion and local random fields to disrupt ferroelectric order and stabilize polar nanoregions, while sluggish diffusion kinetics refine grain morphology and wide-bandgap ions enhance breakdown strength. Consequently, an ultrahigh energy storage performance with Wrec ∼10.72 J cm−3 and η ∼86.9% is achieved at 698 kV cm−1, accompanied by excellent energy storage stability and high hardness (∼8.58 GPa). This work demonstrates that multi-scale high-entropy design is an effective paradigm for developing advanced lead-free energy storage ceramics.
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高影响因子
Nature Communications
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2026
·
IF 18.1
Mu Zhangyan,Ma Zhibin,Zhao Weiyi,Dai Luhan,Xu Dan,Ran Pan,Zhang Panke,Wu Xuejun,Ge Junjie,Ding Mengning
Electrocatalytic alcohol oxidation is pivotal for renewable energy conversion, yet its widespread application is hindered by generally low efficiency, necessitating the development of advanced catalytic systems with boosted electro-oxidation kinetics. In an alkaline electrolyte, the effect of alkali metal cations has been identified as a key impacting factor on the alcohol oxidation activity, but the underlying mechanistic interactions remains insufficiently explored. Here we elucidate the fundamental cation effects on hydroxyl (OH ads ) adsorption and subsequent surface bi-molecular kinetics in Pt (and alloys)-catalyzed alcohol electro-oxidations through combined electrochemical voltammetry, in situ surface enhanced infrared absorption spectroscopy (SEIRAS) and in situ electrical transport spectroscopy (ETS). Systematic evaluations reveal that alkali metal cations regulate the micro-electro-kinetics by modulating the surface coverage of OH ads , which acts bi-functionally as both reactant species and spectator in alcohol oxidations. A matching adsorption kinetics of OH ads and alcohol is key towards the optimal alcohol oxidation activity, providing valuable insights into the cation-mediated alloy catalyst systems and high-concentration conditions in alcohol fuel cells.
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PubMed
高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Hongyang Wang,Chengqi Lu,Pengchang Sun,Zilin Cao,Zhongkang Han,Qianhong Shen,Zhongyuan Hu,Xudan Cao,Hui Yang
A Bi₄Ti₃O₁₂/BiOCl heterojunction with a coherent interface was constructed via a room-temperature ion-exchange process. • A Bi₄Ti₃O₁₂/BiOCl heterojunction with a coherent interface was constructed via a room-temperature ion-exchange process. • The photocatalyst exhibits excellent performance for the degradation of high-concentration, recalcitrant antibiotics. A strategy is reported for the in-situ fabrication of a Bi₄Ti₃O₁₂/BiOCl heterojunction with shared atomic layer through simple room-temperature ion-exchange on pure Bi₄Ti₃O₁₂. This strategic interfacial engineering, combined with a Type-II band alignment, the Aurivillius-type Bi₄Ti₃O₁₂ and BiOCl share the Bi₂O₂ 2+ layers at the interface, thereby dramatically accelerating the separation and migration of photo-generated carriers and ultimately significantly increasing the yield of photocatalytic reactive species. Consequently, the optimized composite photocatalyst exhibits exceptional performance in the degradation of high-concentration antibiotics. It achieves remarkable degradation efficiencies of 90.8% for sulfamethoxazole (20 ppm) within 120 min, 92% for tetracycline hydrochloride (40 ppm) and 78.6% ciprofloxacin (15 ppm) within just 30 min. Demonstrating superior photocatalytic performance compared to the previously reported analogous photocatalysts in recent years with respect to antibiotic degradation. Furthermore, the degradation efficiency of the as-prepared photocatalyst also demonstrates outstanding cycling stability, with a reduction of only 3.4% after 4 cycles. Therefore, this coherent Bi₄Ti₃O₁₂/BiOCl heterojunction photocatalyst exhibits immense potential for practical applications in environmental remediation.
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