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Rational design and energy catalytic application of high-loading single-atom catalysts

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Rare Metals 2024年第10期43卷 4844-4866页

作者： Zi-Wei Deng Yue Liu Jie Lin wen-Xing chen Energy and Catalysis Center School of Materials Science and EngineeringBeijing Institute of Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Science

It is well known that single-atom catalysts(SACs)have become a hot topic in the field of catalysis due to their advantages such as 100% metal atom utilization efficiency,high catalytic activity and selectivity compared with conventional catalysts and nanocatalysts. However, the isolated metal atoms on SACs have thermodynamic instability and tend to agglomerate, which limit their catalytic ***, it is of great significance to synthesize stable and high-loading single-atom catalysts(HLSACs). In this paper,we review the research progress of HLSACs from two aspects:design and application. Firstly, we comprehensively introduce the synthesis strategies of HLSACs, namely, top-down and bottom-up methods. Secondly, we overview the application status of HLSACs in three fields: electrocatalysis, thermal catalysis and photocatalysis. Finally, we summarize the development prospects and challenges of HLSACs.

关键词： Design Electrocatalysis High-loading single-atom catalysts Photocatalysis Thermal catalysis

Experimental observation of the significant difference between surface and bulk Kondo processes in Kondo lattice YbCu_(2)Si_(2)

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Science China(Physics,Mechanics & Astronomy) 2024年第4期67卷 154-160页

作者： Yin-Zou Zhao jiao-jiao Song Qi-Yi Wu Hao Liu chen Zhang Bo chen Hong-Yi Zhang Zhen-Hua chen Yao-Bo Huang Xue-Qing Ye Ya-Hua Yuan Yu-Xia Duan Jun He Jian-Qiao Meng School of Physics Central South UniversityChangsha 410083China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China

Synchrotron-based angle-resolved photoemission spectroscopy was employed to investigate the temperature evolution of the Yb 4 f spectral for surface and bulk in the Kondo lattice YbCu_(2)Si_(2).Our study quantitatively distinguishes between the surface and bulk hybridization processes,revealing that the onset temperatures for both surface and bulk hybridization processes are significantly higher than the Kondo ***,we found that the effective surface Kondo temperature is much lower than that of the *** findings offer valuable insights into the understanding of heavy fermion physics.

关键词： Kondo lattice angle-resolved photoemission spectroscopy electronic structure hybridization surface state

Integrated Stratigraphy and Mineralogy of the Doushantuo Formation in weng’an,South China,and Implications for Ediacaran Phosphogenesis

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Journal of Earth Science 2024年第2期35卷 476-503页

作者： Liangxuan jiao Zhenbing She Dominic Papineau Yaguan Zhang Matthew S.Dodd Kenan Cao Qun chen Guoyong chen State Key Laboratory of Biogeology and Environmental Geology China University of GeosciencesWuhan430078China School of Earth Sciences China University of GeosciencesWuhan430047China London Centre for Nanotechnology University College London17-19 Gordon StreetLondonWC1E 6BTUK Department of Earth Sciences University College LondonLondonWC1E 6BTUK Centre for Planetary Science University College London and Birkbeck CollegeLondonWC1E 7HXUK Innovation Center of Ore Resources Exploration Technology in the Region of Bedrock Ministry of Natural Resources of People’s Republic of China’Guiyang550000China Guizhou Bureau of Geology and Mineral Exploration and Development Guiyang550000China

The Ediacaran–Cambrian Phosphogenic Episode is the Earth’s first true phosphogenic event and resulted in worldwide phosphate deposits,which occurred during the processes of the Neoproterozoic Oxygenation *** Ediacaran Doushantuo Formation(ca.635–551 Ma)of weng’an area in central Guizhou,South China,contains two economic phosphorite beds(the Lower and Upper Phosphorite Beds).This paper presents a detailed stratigraphic,sedimentological and mineralogical study of multiple outcrop and drill core sections of the Doushantuo Formation across the weng’an area,and identified 11 lithofacies and 4 types of phosphatic *** differences in lithofacies and grain types between the upper and lower phosphate deposits are observed,indicating that the two sets of phosphate deposits are the products of two distinct phosphogenic *** Lower Phosphorite Bed mainly consists of banded and laminated phosphorites,contains micro-oncoids formed by microbially-mediated precipitation and peloids formed by in-situ chemically oscillating reactions,indicating a biochemical and chemical enrichment of phosphorus to sediments during the Early Ediacaran *** Upper Phosphorite Bed is mainly composed of carbonaceous,massive,and stromatolitic phosphorites,contains bioclasts(phosphatized spheroidal fossils),and intraclasts formed by hydrodynamic agitation,suggesting that the major accesses of phosphorus to sediments were the remineralization of organic *** of the two economic phosphorite beds was controlled by two sea-level *** differences have also been documented in contemporaneous phosphate-bearing successions in Brazil and Mangolia,indicating a significant shift in global phosphogenic mechanism during the early and middle Ediacaran,which may be due to the changes in redox conditions in seawater,associated with the Neoproterozoic Oxygenation *** regional active P-cycle processes could produce more free oxygen,which may have contributed to the up

关键词： phosphorite lithofacies phosphatic grains phosphogenic paragenesis phosphorus cycle mineralogy

A fungal CYP from Beauveria bassiana with promiscuous steroid hydroxylation capabilities

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Chinese Chemical Letters 2024年第5期35卷 218-222页

作者： Yu Peng Yue Wang Tian-jiao chen Jing-Jing chen Jin-Ling Yang Ting Gong Ping Zhu State Key Laboratory of Bioactive Substance and Function of Natural Medicines NHC Key Laboratory of Biosynthesis of Natural ProductsCAMS Key Laboratory of Enzyme and Biocatalysis of Natural DrugsInstitute of Materia MedicaChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100050China

Hydroxylation of steroid core is critical to the synthesis of steroid *** sp^(3) C-H hydroxylation is challenging through chemical catalysis,alternatively,fungal biotransformation offers a possible solution to this ***,mining and metabolic engineering of cytochrome P450 monooxygenases(CYPs)is usually regarded as a more eco-friendly and efficient ***,we report the mining and identification of a new steroid CYP(CYP68BE1)from Beauveria bassiana by transcriptomics,heterologous expression,in vivo and in vitro functional *** catalytic promiscuity of CYP68BE1 was explored,and CYP68BE1 showed promiscuously and catalytically versatile,which is qualified for monohydroxylation on C11α,C1α,C6βand dihydroxylation on C1β,11αand C6β,11αof six steroids,leading to the production of key steroid intermediates required in the industrial synthesis of some indispensable steroid *** dynamics simulations were performed,revealing the molecular basis of different binding orientations of CYP68BE1 with different *** discovery of CYP68BE1 offers a promising biocatalyst for enriching the steroid structural and functional diversity,which also can be applied to biosynthesize valuable steroid drug intermediates.

关键词： Fungal CYPs Steroid hydroxylase Beauveria bassiana Promiscuous biocatalyst Molecular dynamics

Analysis of Deep Ritz Methods for Semilinear Elliptic Equations

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Numerical Mathematics(Theory,Methods and Applications) 2024年第1期17卷 181-209页

作者： Mo chen Yuling jiao Xiliang Lu Pengcheng Song Fengru Wang Jerry Zhijian Yang School of Mathematics and Statistics Wuhan University299 Ba Yi RoadWuhan 430072P.R.China Hubei Key Laboratory of Computational Science Wuhan University299 Ba Yi RoadWuhan 430072P.R.China

In this paper,we propose a method for solving semilinear elliptical equa-tions using a ResNet with ReLU2 ***,we present a comprehensive formulation based on the penalized variational form of the elliptical *** then apply the Deep Ritz Method,which works for a wide range of *** obtain an upper bound on the errors between the acquired solutions and the true solutions in terms of the depth D,width W of the ReLU2 ResNet,and the num-ber of training samples *** simulation results demonstrate that our method can effectively overcome the curse of dimensionality and validate the theoretical results.

关键词： Semilinear elliptic equations Deep Ritz method ReLUMo ResNet convergence rate

Mo_(2)P Monolayer as a Superior Electrocatalyst for Urea Synthesis from Nitrogen and Carbon Dioxide Fixation:A Computational Study

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Energy & Environmental Materials 2024年第1期7卷 207-214页

作者： Dongxu jiao Zhongxu Wang Yuejie Liu Qinghai Cai Jingxiang Zhao Carlos R.Cabrera Zhongfang chen College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of EducationHarbin Normal UniversityHarbin 150025China Modern Experiment Center Harbin Normal UniversityHarbin 150025China Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety Harbin 150025China Department of Chemistry and Biochemistry The University of Texas at El PasoEl Paso TX 79968USA Department of Chemistry University of Puerto RicoRio Piedras CampusSan JuanPuerto Rico 00931USA

Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather ***,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea *** results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic ***,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side *** outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active *** findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.

关键词： C-N coupling density functional theory Mo_(2)P monolayer urea synthesis

How Do Chinese Exporting Firms Respond to Environment-related Notifications?A Green Innovation Perspective

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China & World Economy 2024年第5期32卷 1-27页

作者： wen chen Yinzi Fan School of Economics Xiamen UniversityChina

Environment-related notifications play an important role in the coordinated development of trade and environment *** this paper,we examine how Chinese exporting enterprises responded to environment-related notifications implemented by the US through green innovation *** notifications significantly encouraged exporting firms to increase green innovation,as evidenced particularly by the number of green utility model patents *** effect was most pronounced in non-foreign-invested enterprises,high-total-factor-productivity firms,technology-intensive industries,and nongreen *** notifications also increased the probability of enterprises exiting the market while reducing the probability of new enterprises entering *** innovation motivation of surviving firms was higher than that of the new *** analysis also suggests that environment-related notifications had a crowding-out effect on other innovation rather than a leverage *** study offers important empirical evidence that helps enterprises to respond to green non-tariff measures effectively,enrich the existing literature,and provide practical guidance for both policymaking and corporate development.

关键词： difference-in-differences environment-related notification green innovation.tradeandenvironment JELcodes:F13 F14 O33

Approaches to sustaining people-place bonds in conservation planning:from value-based,living heritage,to the glocal community

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Built Heritage 2024年第2期8卷 52-66页

作者： Yueyi chen Yi-wen Wang Department of Architecture College of Design and EngineeringNational University of Singapore4 Architecture DriveSingapore117566Singapore Department of Urban Planning&Design Design SchoolXi’an Jiaotong-Liverpool University111 Ren’ai RoadDushu Lake Higher Education TownSuzhou Industrial Park215123Suzhou Industrial ParkChina

This review paper explores approaches to sustaining the enduring connection between communities and heritage places in conservation *** global overtourism,the gradual outmigration and sudden displacement of local communities from heritage places disrupt not only physical ties between people and places but also shared traditions,memories and emotional *** intangible qualities constitute the social dimension of heritage and are pivotal to its cultural ***,existing conservation approaches to safeguarding this social dimension often rely on the continued presence of local communities,which may yield limited effectiveness in restoring people–place bonds amidst challenges posed by overtourism and *** review unpacks the term‘social value’within the framework of value-based assessment and progresses towards a dynamic conception of‘sense of place’.In response to the changing social composition of‘local communities’at heritage places,this review examines approaches for conserving the social dimension of heritage,aiming to sustain the enduring continuity of people–place *** proposes a broader definition of‘sense of place’that transcends the preconceived notion of stakeholder groups as a geographically defined community and suggests leveraging digital social platforms to re-establish these *** review concludes by advocating for the‘glocal community’approach,acknowledging the personal emotional connections that individuals form with a heritage place regardless of their places of *** approach has the potential to complement existing methods,such as value-based assessment and the living heritage approach,which are commonly practised in contemporary conservation efforts.

关键词： social value sense of place continuity conservation area community urban conservation

Construction of wavelength-tunable DSE quinoline salt derivatives by regulating the hybridization form of the nitrogen atom and intramolecular torsion angle

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Chinese Chemical Letters 2024年第10期35卷 315-320页

作者： Kuan Deng Fei Yang Zhi-Qi cheng Bi-wen Ren Hua Liu jiao chen Meng-Yao She Le Yu Xiao-Gang Liu Hai-Tao Feng Jian-Li Li Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory for Carbon Neutral TechnologyCollege of Chemistry&Materials ScienceNorthwest UniversityXi'an710127China Key Laboratory of Resource Biology and Biotechnology in Western China Ministry of EducationBiomedicine Key Laboratory of Shaanxi ProvinceLab of Tissue Engineeringthe College of Life SciencesFaculty of Life Science&MedicineNorthwest UniversityXi'an 710069China Fluorescence Research Group Singapore University of Technology and DesignSingapore 487372Singapore Baoji AIE Research Center Shaanxi Key Laboratory of PhytochemistryCollege of Chemistry and Chemical EngineeringBaoji University of Arts and SciencesBaoji721013China

Dual-state emission(DSE)molecules displayed conspicuous fluorescent performance both in solid and solution ***,the construction of DSE molecules and the regulation of their emission wavelengths remains a great *** on the structure-function relationship of quinolinonitrile-type fluorophores,this work proposed a feasible strategy for modulating their fluorescent properties into DSE via limiting the torsion angle between the quinoline ring and C=C bond in the range of 4.7°to 30°.Based on this strategy,53 compounds were obtained which displayed tunable emission wavelengths from^(3)97 nm to 740 nm in solid-state and from 360 nm to 672 nm in *** feasibility of the strategy was supported by a series of theoretical calculations,optical characterizations,and crystal analysis,suggesting the compounds have great potential in imaging living cells and tissues with desired wavelengths.

关键词： Fluorescence Dual-state emission Structure-function relationship Wavelength regulation Fluorescent imaging