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Engineering atomic Rb-n configurations to tune radical pathways for highly selective photocatalytic H2O2 synthesis coupled with biomass valorization

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Journal of Energy Chemistry 2025年第1期100卷 215-225页

作者： Jiaye Li Shuang Pan Yihuang Chen Qiong liu College of Chemistry and Materials Engineering Wenzhou University Guangdong Provincial Key Laboratory of Chemical Measurement and Emergency Test Technology (China) Institute of Analysis Guangdong Academy of Sciences (China National Analytical CenterGuangzhou)

Photocatalytic oxygen reduction for hydrogen peroxide （H2O2） synthesis presents a green and costeffective production ***,achieving highly selective H2O2synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative ***,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H2O2and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride（CnRb）.The optimized CnRb catalyst demonstrates a record photoreduction rate of 8.01 mM h-1for H2O2generation and photooxidation rate of 3.75 mM h-1for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion （SCC） efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–n configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical *** is because the Rb–n serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product *** study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H2O2coupled with biomass valorization.

关键词： Free radical reactions

Comparative proteomic analysis of plasma exosomes reveals the functional contribution of n-acetyl-alpha-glucosaminidase to Parkinson’s disease

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neural Regeneration Research 2025年第10期20卷 2998-3012页

作者： Yuan Zhao Yidan Zhang Xin liu Jian Zhang Ya Gao Shuyue Li Cui Chang Xiang liu Guofeng Yang Department of Geriatrics Second Hospital of Hebei Medical UniversityShijiazhuangHebei ProvinceChina Department of neurosurgery The Second Hospital of Hebei Medical UniversityShijiazhuangHebei ProvinceChina

Parkinson’s disease is the second most common progressive neurodegenerative disorder,and few reliable biomarkers are available to track disease *** proteins,DnA,mRnA,and lipids carried by exosomes reflect intracellular changes,and thus can serve as biomarkers for a variety of *** this study,we investigated alterations in the protein content of plasma exosomes derived from patients with Parkinson’s disease and the potential therapeutic roles of these proteins in Parkinson’s *** a tandem mass tag-based quantitative proteomics approach,we characterized the proteomes of plasma exosomes derived from individual patients,identified exosomal protein signatures specific to patients with Parkinson’s disease,and identified n-acetyl-alpha-glucosaminidase as a differentially expressed protein.n-acetyl-alpha-glucosaminidase expression levels in exosomes from the plasma of patients and healthy controls were validated by enzyme-linked immunosorbent assay and western *** results demonstrated that the exosomal n-acetyl-alpha-glucosaminidase concentration was not only lower in Parkinson’s disease,but also decreased with increasing Hoehn-Yahr stage,suggesting that n-acetyl-alpha-glucosaminidase could be used to rapidly evaluate Parkinson’s disease ***,western blot and immunohistochemistry analysis showed that n-acetyl-alpha-glucosaminidase levels were markedly reduced both in cells treated with 1-methyl-4-phenylpyridinium and cells overexpressingα-synuclein compared with control ***,n-acetyl-alpha-glucosaminidase overexpression significantly increased cell viability and inhibitedα-synuclein expression in 1-methyl-4-phenylpyridinium-treated *** together,our findings demonstrate for the first time that exosomal n-acetyl-alpha-glucosaminidase may serve as a biomarker for Parkinson’s disease diagnosis,and that n-acetyl-alpha-glucosaminidase may reduceα-synuclein expression and 1-methyl-4-phenylpyridinium-induced n

关键词： biomarker diagnosis exosomes n-acetyl-alpha-glucosaminidase Parkinson’s disease proteomic α-synuclein

Ammonia pyrolysis oxidation excited by nanosecond pulsed discharge:Global/fluid models hybrid solution

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Journal of Energy Chemistry 2025年第1期100卷 385-396页

作者： Mingming Zhang Hanyu Wu Qi Chen Jiaxin Yang Bonan liu School of Mechanical Electronic and Control Engineering Beijing Jiaotong University China University of Petroleum

The kinetic characteristics of plasma-assisted oxidative pyrolysis of ammonia are studied by using the global/fluid models hybrid solution ***,the stable products of plasma-assisted oxidative pyrolysis of ammonia are *** results show that the consumption of nH3/O2and the production of n2/H2change linearly with the increase of voltage,which indicates the decoupling of nonequilibrium molecular excitation and oxidative pyrolysis of ammonia at low ***,the detailed reaction kinetics mechanism of ammonia oxidative pyrolysis stimulated by a nanosecond pulse voltage at low pressure and room temperature is *** on the reaction path analysis,the simplified mechanism is *** detailed and simplified mechanism simulation results are compared with experimental data to verify the accuracy of the simplified ***,based on the simplified mechanism,the fluid model of ammonia oxidative pyrolysis stimulated by the nanosecond pulse plasma is established to study the pre-sheath/sheath behavior and the resultant consumption and formation of key *** results show that the generation,development,and propagation of the pre-sheath have a great influence on the formation and consumption of *** consumption of nH3by the cathode pre-sheath is greater than that by the anode pre-sheath,but the opposite is true for OH and O（1S）.However,within the sheath,almost all reactions do not ***,by changing the parameters of nanosecond pulse power supply voltage,it is found that the electron number density,electron current density,and applied peak voltages are not the direct reasons for the structural changes of the sheath and ***,the discharge interval has little effect on the sheath structure and gas mixture *** research results of this paper not only help to understand the kinetic promotion of non-equilibrium excitation in the process of oxidative pyrolysis but also help to explore th

关键词： nanosecond pulsed discharge Ammonia Oxidative pyrolysis Fluid model Global model

Preparation of FeConi medium entropy alloy from Fe^(3+)-Co^(2+)-ni^(2+)solution system

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 92-101页

作者： Zongyou Cheng Qing Zhao Mengjie Tao Jijun Du Xingxi Huang Chengjun liu Key Laboratory for Ecological Metallurgy of Multimetallic Mineral(Ministry of Education) Northeastern UniversityShenyang 110819China School of Metallurgy Northeastern UniversityShenyang 110819China Engineering Research Center of Frontier Technologies for Low-carbon Steelmaking(Ministry of Education) Shenyang 110819China

In recent years,medium entropy alloys have become a research hotspot due to their excellent physical and chemical *** controlling reasonable elemental composition and processing parameters,the medium entropy alloys can exhibit similar properties to high entropy alloys and have lower *** this paper,a FeConi medium entropy alloy precursor was prepared via sol-gel and coprecipitation methods,respectively,and FeConi medium entropy alloys were prepared by carbothermal and hydrogen *** phases and magnetic properties of FeConi medium entropy alloy were *** showed that FeConi medium entropy alloy was produced by carbothermal and hydrogen reduction at 1500℃.Some carbon was detected in the FeConi medium entropy alloy prepared by carbothermal *** alloy prepared by hydrogen reduction was uniform and showed a relatively high ***,the hydrogen reduction product exhibited better saturation magnetization and lower coercivity.

关键词： medium entropy alloy sol-gel co-precipitation carbothermal hydrogen reduction

Enhanced post-combustion CO2 capture and direct air capture by plasma surface functionalization of graphene adsorbent

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Journal of Energy Chemistry 2025年第1期100卷 653-664页

作者： Rahul navik Eryu Wang Xiao Ding Huang Yunyi Yiyu liu Jia Li Guangdong-Hong Kong Joint Laboratory for Carbon neutrality Jiangmen Laboratory of Carbon and Science and Technology Guangzhou HKUST Fok Ying Tung Research Institute The Hong Kong University of Science and Technology (Guangzhou) Carbon neutrality and Climate Change Thrust Society Hub The Hong Kong University of Science and Technology (Guangzhou) Stoddart Institute of Molecular Science Department of Chemistry Zhejiang University

Graphene has enormous potential to capture CO2due to its unique properties and ***,graphene-based adsorbents have drawbacks of lower CO2adsorption capacity and poor *** work demonstrates a one-step rapid and sustainable n2/H2plasma treatment process to prepare graphene-based sorbent material with enhanced CO2adsorption *** treatment directly enriches amine species,increases surface area,and improves textural *** CO2adsorption capacity increases from 1.6 to 3.3 mmol/g for capturing flue gas,and from 0.14 to 1.3 mmol/g for direct air capture （DAC）.Importantly,the electrothermal property of the plasma-modified aerogels has been significantly improved,resulting in faster heating rates and significantly reducing energy consumption compared to conventional external heating for regeneration of *** aerogels display improved selectivity of 42 and 87 after plasma modification for 5 and 10 min,*** plasma-treated aerogels display minimal loss between 17%and 19% in capacity after 40 adsorption/desorption cycles,rendering excellent *** n2/H2plasma treatment of adsorbent materials would lower energy expenses and prevent negative effects on the global economy caused by climate change.

关键词： Carbon neutrality CO 2 capture Climate change Plasma treatment Graphene aerogel

Co@C-n as an electronic mediator anchored with Cu2O nanoparticles enables efficient photoreduction of CO2 to CO with nearly 100% selectivity

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Science China Chemistry 2025年

作者： Xingbin Pan Xiuzheng Deng Jingshan Fan Jiangchuan liu Changhai liu Zhongyu Li Qian Liang Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology CNPC-CZU Innovation Alliance School of Petrochemical Engineering Changzhou University School of Materials Science & Engineering Changzhou University

Solar-driven CO2conversion into value-added chemical provides an attractive strategy for sustainable development. However,the enhanced CO2photoreduction performance with target product selectivity remains a major challenge. Here, we develop a novel strategy involving Cu2O nanoparticles in situ grown on the surface of ZIF-67-derived Co@C-n nanocages （CC） to create abundant active sites and appropriate heterointerfaces. A remarkable CO selectivity of 95.7%with a yield of 117.39μmol g-1h-1and an apparent quantum efficiency as high as 1.88%at 420 nm was obtained over CC-60 catalyst in pure water, which was 87.6times higher than that of pure Cu2O. Theoretical calculations and experiments indicated that Co@C-n nanocages as charge mediator not only rapidly trap photogenerated electrons to promote charge separation efficiency, but also regulate the d-band center of Cu atoms to move to the Fermi energy level, thereby optimizing the reaction kinetics to facilitate the highly selective conversion of the key intermediate *CO desorption to CO.

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High-dimensional large-scale mixed-type data imputation under missing at random

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Science China Mathematics 2025年

作者： Wei liu Guizhen Li Ling Zhou Lan Luo School of Mathematics Sichuan University Center of Statistical Research and School of Statistics Southwestern University of Finance and Economics Department of Statistics and Actuarial Science University of Iowa

Missingness in mixed-type variables is commonly encountered in a variety of areas. The requirement of complete observations necessities data imputation when a moderate or large proportion of data is ***, inappropriate imputation would downgrade the performance of machine learning algorithms, leading to bad predictions and unreliable statistical inference. For high-dimensional large-scale mixed-type missing data, we develop a computationally efficient imputation method, missing value imputation via generalized factor models（MIG）, under missing at random. The proposed MIG method allows missing variables to be of different types,including continuous, binary, and count variables, and are scalable to both data size n and variable dimension p while existing imputation methods rely on restrictive assumptions such as the same type of missing variables,the low dimensionality of variables, and a limited sample size. We explicitly show that the imputation error of the proposed MIG method diminishes to zero with the rate Op(max{n-1/2, p-1/2}) as both n and p tend to infinity. Five real datasets demonstrate the superior empirical performance of the proposed MIG method over existing methods that the average normalized absolute imputation error is reduced by 5.3%–34.1%.

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Low‑Temperature Oxidation Induced Phase Evolution with Gradient Magnetic Heterointerfaces for Superior Electromagnetic Wave Absorption

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nano-Micro Letters 2025年第1期17卷 191-204页

作者： Zizhuang He Lingzi Shi Ran Sun Lianfei Ding Mukun He Jiaming Li Hua Guo Tiande Gao Panbo liu School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710129People’s Republic of China School of Marine Science and Technology Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China

Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase ***,accordion-shaped Co/Co_(3)O_(4)@n-doped carbon nanosheets(Co/Co_(3)O_(4)@nC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation *** results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial ***,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic ***,the synthesized Co/Co_(3)O_(4)@nC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon *** design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.

关键词： Magnetic heterointerfaces Phase evolution Interfacial polarization Magnetic coupling Electromagnetic wave absorption

Salsolinol as an RnA m~6A methylation inducer mediates dopaminergic neuronal death by regulating YAP1 and autophagy

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neural Regeneration Research 2025年第3期20卷 887-899页

作者： Jianan Wang Yuanyuan Ran Zihan Li Tianyuan Zhao Fangfang Zhang Juan Wang Zongjian liu Xuechai Chen Beijing International Science and Technology Cooperation Base for Antiviral Drugs College of Chemistry and LifeBeijing University of TechnologyBeijingChina Department of Rehabilitation Beijing Rehabilitation HospitalCapital Medical UniversityBeijingChina

Salsolinol(1-methyl-6,7-dihydroxy-1,2,3,4-tetrahydroisoquinoline,Sal)is a catechol isoquinoline that causes neurotoxicity and shares structural similarity with 1-methyl-4-phenyl-1,2,3,6-tetrahydropyridine,an environmental toxin that causes Parkinson's ***,the mechanism by which Sal mediates dopaminergic neuronal death remains *** this study,we found that Sal significantly enhanced the global level of n~6-methyladenosine(m~6A)RnA methylation in PC12 cells,mainly by inducing the downregulation of the expression of m~6A demethylases fat mass and obesity-associated protein(FTO)and alk B homolog 5(ALKBH5).RnA sequencing analysis showed that Sal downregulated the Hippo signaling *** m~6A reader YTH domain-containing family protein 2(YTHDF2)promoted the degradation of m~6A-containing Yes-associated protein 1(YAP1)mRnA,which is a downstream key effector in the Hippo signaling ***,downregulation of YAP1 promoted autophagy,indicating that the mutual regulation between YAP1 and autophagy can lead to *** findings reveal the role of Sal on m~6A RnA methylation and suggest that Sal may act as an RnA methylation inducer mediating dopaminergic neuronal death through YAP1 and *** results provide greater insights into the neurotoxic effects of catechol isoquinolines compared with other studies and may be a reference for assessing the involvement of RnA methylation in the pathogenesis of Parkinson's disease.

关键词： ALKBH5 autophagy FTO Hippo pathway m~6A Parkinson's disease RnA methylation salsolinol YAP1 YTHDF2