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Vacancies-rich CoAl monolayer layered double hydroxide as efficient superoxide dismutase-like nanozyme

Nano Research 2022年第9期15卷 7940-7950页

作者： Shuo Zhang Jun Chen Wen-Sheng Yang Xu Chen State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

With the extensive development of nanozymes in recent years,catalytic efficiency has been considered as the Gordian knot that restricts the further applications of ***,the usage of layered double hydroxides(LDHs)as antioxidant nanozymes for scavenging reactive oxygen species(ROS)has not been ***,we report a vacancies-rich monolayer cobalt-alumina LDH nanosheet(m-CoAl-LDH)through a facile direct synthesis method as an efficient nanozyme with superoxide dismutase(SOD)-like *** m-CoAl-LDH exhibits a record-breaking catalytic efficiency with the catalytic constant(Kcat)as high as 4.33×10^(11)M^(−1)·s−*** by the experimental and theoretical studies,the abundant oxygen and metal vacancies were existed in the single layer for the outstanding performance owing to the increased active *** addition,density functional theory(DFT)calculations further reveal the significant role of synergistic effect of oxygen and metal vacancies in reducing the adsorption energy of superoxide(O_(2)^(•−)),which improves the catalytic *** m-CoAl-LDH nanosheets were applied in cells to relieving the oxidative damage caused by O_(2)^(•−)in *** vacancy-rich monolayer CoAl-LDH nanosheets represent the first example of LDH nanozyme with specific SOD-like activity as well as record high catalytic efficiency,which may provide deeper insight into efficient nanozyme design by defect-engineering.

关键词： nanozymes superoxide dismutase layered double hydroxides defect catalytic efficiency

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Sustainable Carbon-Based Catalyst Materials Derived From Lignocellulosic Biomass for Energy Storage and Conversion: Atomic Modulation and Properties Improvement

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Carbon Energy 2025年第5期7卷 59-104页

作者： Wei Li Ying Xu Guanhua Wang Ting Xu Kui Wang Shangru Zhai Chuanling Si State Key Laboratory of Biobased Fiber Manufacturing Technology Tianjin Key Laboratory of Pulp and Paper College of Light Industry and EngineeringTianjin University of Science and Technology Institute of Chemical Industry of Forest Products Chinese Academy of Forestry Key Laboratory of Biomass Energy and Material School of Environmental and Nature Resources Zhejiang University of Science & Technology

Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components, various dimensions, high carbon content, and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently. Due to the catalytic deficiency of neutral carbon atoms, the usage of single lignocellulosic-based carbon materials in electrocatalysis involving energy storage and conversion presents unsatisfactory applicability. However, atomic-level modulation of lignocellulose-based carbon materials can optimize the electronic structures, charge separation, transfer processes, and so forth,which results in substantially enhanced electrocatalytic performance of carbon-based catalysts. This paper reviews the recent advances in the rational design of lignocellulosic-based carbon materials as electrocatalysts from an atomic-level perspective,such as self/external heteroatom doping and metal modification. Then, through systematic discussion of the design principles and reaction mechanisms of the catalysts, the applications of the prepared lignocellulosic-based catalysts in rechargeable batteries and electrocatalysis are reviewed. Finally, the challenges in improving the catalytic performance of lignocellulosicbased carbon materials as electrocatalysts and the prospects in diverse applications are reviewed. This review contributes to the synthesis strategy of lignocellulose-based carbon electrocatalysts via atomic-level modulation, which in turn promotes the lignocellulose valorization for energy storage and conversion.

关键词： atomic modulation carbon materials electrocatalysis lignocellulosic biomass rechargeable batteries

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Hierarchical CoNi-LDH nanosheet array with hydrogen vacancy for high-performance aqueous battery cathode

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Journal of Energy Chemistry 2022年第6期31卷 9-15,I0001页

作者： Wang Qiao Bowen Jin Wenfu Xie Mingfei Shao Min Wei State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Aqueous rechargeable multiple metal-ion storage battery (ARSB) has a large potential in energy storage devices due to their safe usage, low cost and high rate capability. Nevertheless, the performance of practical ARSB is largely restricted by low capacity and limited cathode materials. Herein, we demonstrate an efficient cathode material based on Co Ni-layered double hydroxide (LDH) nanosheets arrays with abundant hydrogen vacancy induced by electrochemical activation process for high performance of cations storage. Consequently, the electrochemical activated Co Ni-LDH (ECA-Co Ni-LDH) nanosheets arrays exhibit high metal ion (Li^(+), Na^(+), Zn^(2+), Mg^(2+) and Ca^(2+)) storage capacities, which is 9 times and 3 times higher that of unactivated Co Ni-LDH arrays and ECA-Co Ni-LDH without hierarchical structure, ***, the ECA-Co Fe-LDH also shows the possibility for practical applications in actual *** coupling with a Fe_(2)O_(3)/C anode, the assembled aqueous battery delivered a large energy density of 184.4 Wh kg^(-1)at power density of 4 Wh kg^(-1) in high voltage range of 0–2 V. To our best knowledge, such high energy density and large working window of our assembled aqueous battery is exceeded other LDH-based aqueous battery or supercapacitor, and the energy density almost comparable than that of commercial Li-ion batteries. Moreover, almost no measurable capacitance losses can be detected even after 10000 cycles. In addition, this work also provides a strategy to develop a high energy density cathode for multiple metal-ion storage batteries.

关键词： Layered double hydroxides Multiple ions intercalation Hierarchical structure Hydrogen vacancy Aqueous battery

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Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge:The performance and absorption mechanism

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Chinese Journal of chemical engineering 2024年第1期65卷 212-221页

作者： Yuanyuan Yin Xujun Wang Lei Xu Binbin He Yunxiang Nie Yi Mei Faculty of Chemical Engineering Kunming University of Science and TechnologyKunming 650500China Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials Kunming 650500China The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan Province Kunming 650500China

Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially for small and medium-sized coal-fired boilers and ***,phosphorus sludge,an industrial waste from the production process of yellow phosphorus,has been developed to simultaneously eliminate SO_(2)and NO_(x)from coal-fired flue *** key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95%can be achieved at a low temperature of 55℃.Further,the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption *** efficient removal of SO_(2)is attributed to the abundance of iron(Fe^(3+))and manganese(Mn^(2+))in the ***_(2)can be rapidly catalyzed and converted to SO_(4)^(2-)by *** key to NOx removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus,which are then absorbed by water and converted to NO_(3)^(-).Meanwhile,yellow phosphorus is oxidized to phosphoric acid(H_(3)PO_(4)).The spent absorption slurry can be reused through wet process phosphoric acid production,as it contains sulfuric acid(H_(2)SO_(4)),nitric acid(HNO_(3)),and H_(3)PO_(4).Accordingly,this is a technology with broad application prospects.

关键词： Absorption Oxidation Multiphase reaction Phosphorus sludge Yellow phosphorus Low temperature

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Cystine-assisted accumulation of gold nanoparticles on ZnO to construct a sensitive surface-enhanced Raman spectroscopy substrate

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Frontiers of chemical Science and engineering 2023年第1期17卷 15-23页

作者： Qi Qu Chuan Zeng Jing Huang Mengfan Wang Wei Qi Zhimin He School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300072China School of Life Sciences Tianjin UniversityTianjin 300072China Co-Innovation Centre of Chemistry and Chemical Engineering of Tianjin Tianjin 300072China Tianjin Key Laboratory of Membrane Science and Desalination Technology Tianjin 300350China Technical Centre of Gongbei Customs District of China Zhuhai 519000China

Recently,various semiconductor/metal composites have been developed to fabricate surfaceenhanced Raman spectroscopy ***,low metal loading on semiconductors is still a *** this study,cystine was introduced to increase the accumulation of gold nanoparticles on zinc oxide,owing to the biomineralization_property of_*** analysis revealed that the obtained ZnO/Au/cystine composite not only had a higher metal loading but also formed a porous structure,which is beneficial for Raman *** with ZnO/Au,the ZnO/Au/cystine substrate displayed a 40-fold enhancement in the Raman signal and a lower limit of detection(10^(-11) mol·L^(-1))in the detection of rhodamine ***,the substrate has favorable homogeneity and ***,ZnO/Au/cystine displayed excellent performance toward crystal violet and methylene blue in a test based on river water *** study provided a promising method to fabricate sensitive semiconductor/noblemetal-based surface-enhanced Ramans spectroscopy substrates for Raman detection.

关键词： biomineralization cystine semiconductor/metal composite SERS detection Raman detection

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Exploring the role of cationic lipids in modulating immunogenicity and vaccine efficacy of mRNA-LNP

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Particuology 2025年第2期97卷 1-11页

作者： Yan Zhou Xiangfei Shan Renji Gu Yufei Xia Xiaonan Huang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100081China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing10090China

The mRNA vaccines have become a transformative platform in medicine,with their success during the COVID-19 pandemic accelerating research in viral prevention and cancer *** nanoparticles(LNPs)enhance the stability and efficacy of mRNA vaccines,but achieving an optimal balance between innate immune activation and mRNA expression is crucial for their *** cationic lipids,although largely replaced by ionizable lipids due to concerns over excessive immunogenicity,have demonstrated potential in cancer immunotherapy by inducing strong immune *** this study,we investigated whether incorporating cationic lipids into mRNA-LNP formulations could enhance immunogenicity without requiring new lipid *** introduced varying proportions of cationic lipids into D-Lin-MC3-DMA and SM-102-based LNPs and evaluated their impact on innate immune activation,along with long-term humoral and cellular immune *** results showed that in MC3-based LNPs,cationic lipids significantly improved anti-tumor efficacy,though slightly diminished long-term humoral and cellular *** contrast,in SM-102-based LNPs,cationic lipids enhanced anti-tumor effects without negatively impacting long-term *** findings suggest that adding cationic lipid as an additional component allows for the fine-tuning of mRNA-LNP immunogenicity,expanding the potential applications of mRNA vaccines and simplifying LNP design.

关键词： Lipid nanoparticle mRNA vaccine Immunogenicity Cationic lipids Immune response

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High concentration of Ti^(3+)in C-TiO_(x)nanosheets boosting efficient photodegradation

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Science China(Technological Sciences) 2025年第3期68卷 156-166页

作者： Chongbei WU Xuan LI Haibin WANG Jiaxin TANG Shuai WEI Yuanyuan WU Aobing WANG Jizhou JIANG Hebei Key Laboratory of Man-machine Environmental Thermal Control Technology and Equipment Hebei Vocational University of Technology and EngineeringXingtai054000China School of Materials Science and Engineering Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan430205China

Semiconductor photocatalysis holds significant promise for addressing dye-pollution in ***,the efficiency of photocatalytic water purification is constrained by the weak light absorption capacity and low active site distribution of *** a bottom-up approach,carbon-doped TiO_(x)(C-TiO_(x))nanosheets with high concentrations of Ti^(3+)active sites were fabricated by etching the Al element in Ti_(3)Ai C_(2)with H_(2)O_(2).Experimental evidence demonstrates that the optimal C-TiO_(x)nanosheets exhibit high activity for the photocatalytic degradation of methylene blue,achieving a degradation rate of 100%within 50 *** introduction of carbon into the C-TiO_(x)nanosheets induces a red shift in the absorption edge,boosting the migration of photo-generated charge ***,there is a significant correlation between the concentration of Ti^(3+)active sites and the density of oxygen vacancies in the C-TiO_(x)nanosheets,which synergistically influence the photocatalytic degradation performance of MB dye wastewater.

关键词： bottom-up strategies C-TiO_(x)nanosheets high-concentrations Ti^(3+) photocatalytic degradation

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Micromixing efficiency and enhancement methods for non-Newtonian fluids in millimeter channel reactors

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Chinese Journal of chemical engineering 2025年第2期78卷 108-119页

作者： Zhaoyi Song Yuanxi Zhang Guangwen Chu Lei Shao Yang Xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Research Center of the Ministry of Education for High Gravity Engineering and Technology Beijing University of Chemical TechnologyBeijing 100029China

Millimeter channel reactors(MCRs)have received increasing attention because of their ability to enhance treatment capacity in addition to the advantages of *** previous studies,less work has been conducted on the micromixing process and enhancement strategies for non-Newtonian fluids in *** this study,the micromixing efficiency in MCRs was experimentally investigated using CMC(carboxymethyl cellulose sodium)aqueous solution to simulate a non-Newtonian fluid,and the enhanced mechanism of micromixing efficiency by the addition of internals and rotation was analyzed by computational fluid dynamics(CFD)*** results show that in the conventional channel,increasing the flow rate improves the micromixing efficiency when the CMC concentration is ***,when the CMC concentration is higher,the higher the flow rate,the lower the micromixing *** highest micromixing efficiency is obtained for the rotationally coupled inner components,followed by the single rotation and the lowest is for the internals *** simulations reveal that the most effective way to improve the micromixing efficiency of non-Newtonian fluids with shear-thinning behavior is to increase the shear force in the reactor,which effectively reduces the apparent *** results provide the theoretical foundation for enhancing the micromixing process of non-Newtonian fluids in small-size reactors.

关键词： Millimeter channel Micromixing CFD Viscous Non-Newtonian fluid

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Hybrid HMX multi-level assembled under the constraint of 2D materials with efficiently reduced sensitivity and optimized thermal stability

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Defence technology（防务技术） 2024年第9期39卷 123-132页

作者： Xiaomin Song Longjin Huang Rufang Peng Qi Huang Jinjiang Xu Jie Sun Institute of Chemical Materials China Academy of Engineering PhysicsMianyang621900China State Key Laboratory of Environment-friendly Energy Materials School of Materials Science and EngineeringSouthwest University of Science and TechnologyMianyang621010China

The interfacial interaction between HMX molecules and coating materials is the key to the safety performance of explosives and has received extensive ***,screening suitable coating agents to enhance the interfacial effect to obtain high-energy and low-sensitivity explosives has long been a major *** this work,HMX-PEI/rGO/g-C_(3)N_(4)(HPrGC)composites were innovatively prepared by a multi-level coating strategy of two-dimensional graphite rGO and g-C_(3)N_(4).The g-C_(3)N_(4) used for desensitization has a richπ-conjugated system and shows outstanding ability in reducing friction *** hierarchical structure of HPrGC formed by electrostatic self-assembly andπ-πstacking can effectively dissipate energy accumulation under heat and mechanical stimulation through structural evolution,thus exhibiting a prominent synergistic desensitization effect on *** results show that rGO/gC_(3)N_(4) coating has no effect on the crystal structure and chemical structure of *** importantly,the perfect combination of g-C_(3)N_(4) and rGO endows HPrGC with enhanced thermal stability and ideal mechanical sensitivity(IS:21 J,FS:216 N).Obviously,the new fabrication of HPrGC enriches the variety of desensitizer materials and helps to deepen the understanding of the interaction between explosives and coatings.

关键词： HMX-PEI/rGO/g-C_(3)N_(4) Electrostatic self-assembly π-πstacking Synergistic desensitization

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Promotion effect of epoxy group neighboring single-atom Cu site on acetylene hydrochlorination

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Chinese chemical Letters 2024年第6期35卷 258-262页

作者： Junchen Peng Xue Yin Dandan Dong Zhongyuan Guo Qinqin Wang Minmin Liu Fei He Bin Dai Chaofeng Huang School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832000China College of Chemistry&Chemical Engineering Yantai UniversityYantai 264010China School of Material Science and Engineering University of JinanJi’nan 250022China

Carbon materials have been used as the support for catalysts in the field of acetylene hydrochlorination,the influence of inevitable oxygen-containing moieties on the reaction is often ignored and the mechanism of the oxygen-doping structure remains ***,we explored the effect of the oxygen-containing group(C-O-C)in the support on the activity of single-atom dispersed Cu *** immersing the Cu single-atom catalyst in an alkaline solution,the epoxy species on the carbon support was cleaved to obtain a pure ether species while the Cu site was modified to a more electron-deficient *** turnover frequency value of Cu/O-FLP catalyst with epoxy groups was 1.6-fold higher than that of alkaline treated *** result indicated that the epoxy groups could assist adjacent single-atom Cu sites to synergistically promote the adsorption and cleavage of the reactant hydrogen chloride toward form C-OH and Cu-Cl bonds,and reduce the reaction energy *** presence of electron deficient Cu sites and ether species could induce competitive adsorption of the acetylene and hydrogen chloride,thereby reducing the activity of the *** study highlights the influence of surface oxygen species and the tunability of the support,providing the foundation for the fabrication of higher-activity Cu catalysts for acetylene hydrochlorination.

关键词： Epoxy group Acetylene hydrochlorination Single-atom Cu catalyst Synergistic dissociation

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