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Selective Hydrodeoxygenation of Lignin-Derived Vanillin via Hetero-Structured High-Entropy Alloy/Oxide Catalysts

Energy & Environmental Materials 2024年第3期7卷 202-210页

作者： Yan Sun Kaili Liang Ren Tu Xudong Fan Charles Q.jia Zhiwen jia Yingnan Li Hui Yang Enchen jiang Hanwen Liu Yonggang Yao Xiwei Xu Key Laboratory for Biobased Materials and Energy of Ministry of Education College of Materials and EnergySouth China Agricultural UniversityGuangzhou 510640China Department of Chemical Engineering and Applied Chemistry University of Toronto200 College StreetToronto ON M5S3E5Canada State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added *** their complex molecular structures often require multiple active sites synergy for effective activation and achieving high ***,it is reported that a high-entropy alloy(HEA)on high-entropy oxide(HEO)hetero-structured catalyst for highly active,chemoselective,and robust vanillin *** heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs(niZnCuFeAlZrO_(x)),where exsolvable metals(e.g.,ni,Zn,Cu)in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO *** catalyst exhibits excellent catalytic performance:100%conversion of vanillin and 95%selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120℃,which were attributed to the synergistic effect among HEO matrix(with abundant oxygen vacancies),anchored HEA nanoparticles(having excellent hydrogenolysis capability),and their intimate hetero-interfaces(showing strong electron transferring effect).Therefore,our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion,which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.

关键词： biomass conversion heterogeneous catalysts high-entropy oxide high-entropy alloys lignin pyrolysis

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Heteroatom anchors Fe-Mn dual-atom catalysts with bi-functional oxygen catalytic activity for low-temperature rechargeable flexible Zn-air batteries

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Journal of Energy Chemistry 2024年第3期90卷 610-620,I0014页

作者： Yuting He Hongtao Li Yi Wang Yufei jia Yongning Liu Qiang Tan State Key Laboratory for Mechanical Behaviour of Materials School of Materials Science&EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

M-N-C(M=Fe,Co,ni,etc.) catalyst owns high catalytic activity in the oxygen catalytic reaction which is the most likely to replace the Pt-based *** it is still a challenge to further increase the active site *** article constructs the high-efficiency FeMn-N/S-C-1000 catalyst to realize ORR/OER bifunctional catalysis by hetero-atom,bimetal(Fe,Mn) doped simultaneously *** evaluated it as bi-functional electro-catalysts,FeMn-N/S-C-1000 exhibits excellent catalytic activity(E_(1/2)=0.924 V,E_(j=10)=1.617 V) in alkaline media,outperforms conventional Pt/C,RuO_(2) and most non-precious-metal catalysts reported recently,Such outstanding performance is owing to N,S co-coordinated with metal to form multi-types of single atom,dual atom active sites to carry out ***,nitrite poison test provides the proof that the active sites of FeMn-N/S-C are more than that of single-atom catalysts to promote catalytic reactions *** better understand the local structure of Fe and Mn active sites,XAS and DFT were employed to reveal that FeMn-N_5/S-C site plays the key role during ***,the FeMn-N/S-C-1000 based low-temperature rechargeable flexible Zn-air also exhibits superior discharge performance and extraordinary durability at-40℃.This work will provide a new idea to design diatomic catalysts applied in low-temperature rechargeable batteries.

关键词： Fe Mn-N/S-C-1000 ORR OER Rechargeable flexible Zn-air batteries

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Predication of Selective Ring-opening Hydrogenolysis for Furfuryl Alcohol to Produce Pentanediol over Dual-atom Catalysts

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Chemical Research in Chinese Universities 2024年第1期40卷 55-63页

作者： WANG Tingting WANG jia XI Yongjie HU Bin LI Fuwei State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

Selective activation of C-O bond is of fundamental importance in the precise conversion of oxygenates into value-added compounds in an atom-economic and sustainable manner, and meanwhile, the structurally well-defined dual-atoms catalysts (DACs) have been scarcely investigated in this field. In this study, a series of transition metal DACs anchored on nitrogen-doped graphene (TM2/NC, TM=Pt, Ir, Rh, Pd, Ru, Co, ni and Cu) was constructed to make a comprehensive investigation of their selectivity in the hydrogenative transformation of furfuryl alcohol (FAL), an important biomass platform molecule, to 1,2-pentanediol (1,2-PeD) via selective cleavage of furanic C5-O bond, by density functional theory (DFT) calculations and microkinetic modeling. We found that Ir2/NC demonstrated a high selectivity for the cleavage of furanic C5-O bond to produce 1,2-PeD, while the production of THFAL or 1,5-pentanediol (1,5-PeD) on other TM2/NC catalysts are more favorable. Furthermore, we found that the selective C-O bond cleavage of FAL furan ring is affected by the orbital overlap between the d-orbitals of the anchored metal atoms and the p-orbitals of the adsorbed C atom in FAL, suggesting that the selectivity of the C-O bond cleavage is inextricably related with the electronic property of the anchored metals.

关键词： Furfuryl alcohol Hydrogenation Dual-atom catalyst Density functional theory(DFT)calculation

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Tribological Behaviors of Electroless nickel-Boron Coating on Titanium Alloy Surface

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Chinese Journal of Mechanical Engineering 2024年第1期37卷 309-320页

作者： Yao jia jianping Lai jiaxin Yu Huimin Qi Yafeng Zhang Hongtu He Key Laboratory of Testing Technology for Manufacturing Process in Ministry of Education State Key Laboratory of Environment-Friendly Energy MaterialsSouthwest University of Science and TechnologyMianyang 621010China

Titanium alloys are excellent structural materials in engineering fields,but their poor tribological properties limit their further *** plating is an effective method to enhance the tribological performance of alloys,but it is difficult to efficiently apply to titanium alloys,due to titanium alloy’s strong chemical *** this work,the electroless nickel-Boron(ni-B)coating was successfully deposited on the surface of titanium alloy(Ti-6AL-4V)via a new pre-treatment ***,linearly reciprocating sliding wear tests were performed to evaluate the tribological behaviors of titanium alloy and its electroless ni-B *** was found that the ni-B coatings can decrease the wear rate of the titanium alloy from 19.89×10^(−3)mm^(3)to 0.41×10^(−3)mm^(3),which attributes to the much higher hardness of ni-B *** heat treatment,the hardness of ni-B coating further increases corresponding to coating crystallization and hard phase ***,heat treatment does not improve the tribological performance of ni-B coating,due to the fact that higher brittleness and more severe oxidative wear exacerbate the damage of heat-treated ***,the ni-B coatings heat-treated both in air and nitrogen almost present the same tribological *** finding of this work on electroless coating would further extend the practical applications of titanium alloys in the engineering fields.

关键词： Electroless coating Titanium alloy Tribology Wear Heat treatment Nanoindentation

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Asymmetric radical allylation of β-keto esters with vinyl cyclopropanes by dual photoredox/nickel catalysis

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Science China Chemistry 2024年第11期67卷 3807-3816页

作者： Wen-Yuan Qu Xue-Song Zhou Wen-Jing Xiao jia-Rong Chen Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of EducationCollege of Chemistry Central China Normal University Wuhan Institute of Photochemistry and Technology Key Laboratory of Organo-Pharmaceutical Chemistry of jiangxi Province Gannan Normal University

Radical-involved allylation reactions have emerged as a powerful platform for construction of carbon-carbon and carbonheteroatom bonds, facilitating the strategic incorporation of diverse allyl moieties. Nevertheless, this burgeoning field still faces ongoing challenges, including limitations of radical precursors and coupling partners, and difficulties in achieving enantiocontrol. Herein, we report for the first time a highly enantioselective radical allylation involving β-keto esters with vinyl cyclopropanes utilizing a synergistic dual photoredox/nickel catalysis under visible light irradiation. The mild and redox-neutral catalytic protocol demonstrates an extensive substrate compatibility and good functional tolerance, providing access to enantioenriched β-keto esters featuring quaternary α-stereocenter with good yields and high enantioselectivities. Preliminary mechanistic studies have uncovered that the success of the reaction hinges on the dual roles of nickel catalyst, including in situ formation of photoredox sensitive substrate/ni complex and the ensuing asymmetric radical addition step.

关键词： asymmetric allylation photoredox catalysis radical addition nickel catalysis β-keto esters vinyl cyclopropanes

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诠释取向的叙事政策分析:回顾、反思与重构

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学习论坛 2024年第2期 74-82页

作者：李亚贾鑫王倪北京航空航天大学公共管理学院北京100191 上海交通大学国际与公共事务学院上海200030

面对中国场景下的政策争议,叙事政策分析展现出了潜在优势。基于诠释和实证两种取向叙事政策分析的梳理,评述其研究现状及理论价值,发现诠释取向的叙事政策分析有突出的理论价值,但在服务于政策咨询方面仍存在局限,具体表现为政策叙事... 详细信息

面对中国场景下的政策争议,叙事政策分析展现出了潜在优势。基于诠释和实证两种取向叙事政策分析的梳理,评述其研究现状及理论价值,发现诠释取向的叙事政策分析有突出的理论价值,但在服务于政策咨询方面仍存在局限,具体表现为政策叙事结构与要素不清晰、分析过程的参与不足以及分析结果止步于议题重构。基于此,面向冲突情境下的政策制定需求,尝试构建一套诠释取向的叙事政策分析新方案:在细化政策叙事结构与要素的基础上,将其与深度的参与或协商相结合,以参与式互动为核心,构建面向未来行动方案的元叙事,以支持政策争议的分析与化解。

关键词：政策争议叙事政策分析诠释协商互动

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A genomic association study revealing subphenotypes of childhood steroid-sensitive nephrotic syndrome in a larger genomic sequencing cohort

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Genes & Diseases 2024年第4期11卷 400-410页

作者： Han Chan Fenfen ni Bo Zhao Huimin jiang Juanjuan Ding Li Wang Xiaowen Wang Jingjing Cui Shipin Feng Xiaojie Gao Xueying Yang Huan Chi Hao Lee Xuelan Chen Xiaoqin Li jia jiao Daoqi Wu Gaofu Zhang Mo Wang Yupeng Cun Xiongzhong Ruan Haiping Yang Qiu Li Department of Nephrology Children's Hospital of Chongqing Medical UniversityNational Clinical Research Center for Child Health and DisordersMinistry of Education Key Laboratory of Child Development and DisordersChongqing Key Laboratory of PediatricsChongqing 400014China Department of Nephrology Shenzhen Children's HospitalShenzhenGuangdong 518034China Department of Nephrology Kunming Children's HospitalKunming Medical UniversityKunmingYunnan 650228China Department of Nephrology Wuhan Children's HospitalTongji Medical College of Huazhong University of Science and TechnologyWuhanHubei 430015China Department of Nephrology Chengdu Women and Children Central HospitalChengduSichuan 610073China Pediatric Research Institute Ministry of Education Key Laboratory of Child Development and DisordersNational Clinical Research Center for Child Health and DisordersChina International Science and Technology Cooperation Base of Child Development and Critical DisordersChongqing Key Laboratory of Translational Medical Research in Cognitive Development and Learning and Memory DisordersChildren's Hospital of Chongqing Medical UniversityChongqing 400014China Department of Nephrology John Moorhead Research LaboratoryUniversity College London Medical SchoolRoyal Free CampusUniversity College LondonLondon NW32PFUnited Kingdom

Dissecting the genetic components that contribute to the two main subphenotypes of steroid-sensitive nephrotic syndrome(SSNS)using genome-wide association studies(GWAS)strategy is important for understanding the *** conducted a multicenter cohort study(360 patients and 1835 controls)combined with a GWAS strategy to identify susceptibility var-iants associated with the following two subphenotypes of ssNS:steroid-sensitive nephrotic syn-drome without relapse(SSNswR,181 patients)and steroid-dependent/frequent relapse nephrotic syndrome(SDNS/FRNS,179 patients).The distribution of two single-nucleotide poly-morphisms(SNPs)in ANKRD36 and ALPG was significant between SSNSWR and healthy controls,and that of two SNPs in GAD1 and HLA-DQA1 was significant between SDNS/FRNS and healthy ***,rs1047989 in HLA-DQA1 was a candidate locus for SDNS/FRNS but not for *** significant SNPs were observed between SSNSWR and SDNS/***,chromosome 2:171713702 in GAD1 was associated with a greater steroid dose(>0.75 mg/kg/d)upon relapse to first remission in patients with SDNS/FRNS(odds ratio=3.14;95%confidence interval,0.97-9.87;P=0.034).rs117014418 in APOL4 was significantly associated with a decrease in eGFR of greater than 20%compared with the baseline in SDNS/FRNS patients(P=0.0001).Protein-protein intersection network construction suggested that HLA-DQA1 and HLA-DQB1 function together through ***,SSNSWR belongs to non-HLA region-dependent nephropathy,and the HLA-DQA/DQB region is likely strongly associated with dis-ease relapse,especially in SDNS/*** study provides a novel approach for the GWAS strategy of SsNS and contributes to our understanding of the pathological mechanisms of SSNSWRandSDNS/FRNS.

关键词： Frequentrelapse Genome-wide association study Human leukocyte antigen region Steroid-sensitive nephrotic syndrome

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媒介化视阈下人工智能艺术创作的本质探究与价值阐释

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现代传播（中国传媒大学学报） 2024年第8期46卷 95-103页

作者：倪万郭嘉良山东大学新闻传播学院

从基于媒介技术形态的创新性定位而言,人工智能技术的应用不是对现行艺术创作价值体系的颠覆,而是对既有艺术创作模式与生产要素关系的延续,其技术形态仍然属于工具创新范畴。从人机学习与艺术创作的本质性区别而言,将算法与数据作为底... 详细信息

从基于媒介技术形态的创新性定位而言,人工智能技术的应用不是对现行艺术创作价值体系的颠覆,而是对既有艺术创作模式与生产要素关系的延续,其技术形态仍然属于工具创新范畴。从人机学习与艺术创作的本质性区别而言,将算法与数据作为底层逻辑的人工智能技术,在艺术的知识创作过程中并不具有主体性地位。作为预设的程序框架与重组的数据序列,人工智能的艺术生产机制仍是对人类经验与情感的结构化模拟。从媒介技术对于艺术文化的建构作用而言,人类社会应抵制人工智能技术对艺术创作的规范性宰制,应在技术与艺术的融合语境下,保有艺术创作的自主性与文化形式的多样性。

关键词：深度媒介化人工智能技术形态主体性艺术价值

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Bimetallic Coni single atoms supported on three-dimensionally ordered mesoporous chromia:highly active catalysts for n-hexane combustion

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Green Energy & Environment 2024年第7期9卷 1122-1137页

作者： Xiuqing Hao Yuxi Liu Jiguang Deng Lin Jing jia Wang Wenbo Pei Hongxing Dai Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing100124China

Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and ni single-atom(Co_(1)ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and ni nanoparticle(Co_(NP)ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,*** results indicate that the Co_(1)ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.

关键词： Three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt-nickel single atoms n-Hexane combustion Catalytic reaction mechanism

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Evolution of microstructure and properties of a novel ni-based superalloy during stress relief annealing

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International Journal of Minerals,Metallurgy and Materials 2024年第8期31卷 1876-1889页

作者： Lei jia Heng Cui Shufeng Yang Shaomin Lü Xingfei Xie Jinglong Qu Collaborative Innovation Center of Steel Technology University of Science and Technology BeijingBeijing 100083China State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China Beijing GAONA Materials&Technology Co. Ltd.Beijing 100081China High-Temperature Materials Institute Central Iron and Steel Research InstituteBeijing 100081China

We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resolution transmission electron microscopy(HRTEM),and electron backscatter diffraction(EBSD).The findings reveal that annealing processing has a significant impact on diminishing residual *** the annealing temperature rose from 950 to 1150℃,the majority of the residual stresses were relieved from 60.1 MPa down to 10.9 ***,the stress relaxation mechanism transitioned from being mainly controlled by dislocation slip to a combination of dislocation slip and grain boundary ***,the annealing treatment promotes the decomposition of the Laves,accompanied by the precipitation ofμ-(Mo_(6)Co_(7))starting at 950℃ and reaching a maximum value at 1050℃.The tensile strength and plasticity of the annealing alloy at 1150℃ reached the maximum(1394 MPa,56.1%)which was 131%,200%fold than those of the as-cast alloy(1060 MPa,26.6%),but the oxidation process in the alloy was accelerated at 1150℃.The enhancement in durability and flexibility is primarily due to the dissolution of the brittle phase,along with the shape and dispersal of theγ′phase.

关键词： GH4151 alloy annealing treatment residual stress precipitation evolution strength mechanical properties

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