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Identification of the optimal doping position of hetero-atoms in chalcogen-doped Fe-N-C catalysts for oxygen reduction reaction

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Particuology 2024年第6期89卷 99-108页

作者： Weihao Liu Huanhuan he Qingtao Liu Xin wan Jianglan Shui School of Materials Science and Engineering Beihang UniversityBeijing100191China School of Space and Environment Beihang UniversityBeijing102206China Tianmushan Laboratory Hangzhou310023China

The excellent oxygen reduction reaction(ORR)activity of Fe–N–C catalysts in acidic media makes them potential for low-cost proton exchange membrane fuel *** recent years,it has been shown that heteroatoms(B,O,S,P,Cl,F,etc.)can be used as electron-withdrawing groups to modulate the planar structure and electron distribution of the Fe–Nx active sites to achieve simultaneous improvement of catalytic activity and ***,the optimal location of the heteroatoms remains ***,taking chalcogen heteroatoms(S and Se)as an example,we control the doping positions and investigate their effect on the ORR performance of the Fe–N–C *** first coordination shell of the iron single atom is identified as the optimal doping *** optimized catalysts Fe–N_(3)Se_(1)/NC and Fe–N_(3)Se_(1)/NC demonstrate improved activity and stability in both half cells and fuel *** work provides insights into the enhancement mechanism of heteroatom doping in single-atom catalysts.

关键词： Oxygen reduction reaction Fe-N-C catalysts hetero-atom doping Doping position Enhancement mechanism

Electrochemical synthesis of trimetallic nickel-iron-copper nanoparticles via potential-cycling for high current density anion exchange membrane water-splitting applications

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Journal of Energy Chemistry 2024年第2期89卷 535-542,I0012页

作者： Ziqi Zhang Sheng wan Hanbo wang Jinghan he Ruige Zhang Yuhang Qi Haiyan Lu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina

Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil *** water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity ***,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment ***,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel *** synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline ***,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.

关键词： Electrocatalytic water splitting Hydrogen evolution reaction Oxygen evolution reaction Electrochemical synthesis Anion exchange membrane

Excessive manure application stimulates nitrogen cycling but only weakly promotes crop yields in an acidic Ultisol:Results from a 20-year field experiment

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Journal of Integrative Agriculture 2024年第7期23卷 2434-2445页

作者： Song wan Yongxin Lin Hangwei Hu Milin Deng Jianbo Fan Jizheng he Key Laboratory for Humid Subtropical Eco-geographical Processes of Ministry of Education School of Geographical Sciences/School of Carbon Neutrality Future TechnologyFujian Normal UniversityFuzhou 350007China School of Agriculture and Food Faculty of ScienceThe University of MelbourneParkvilleVictoria 3010Australia State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil ScienceChinese Academy of SciencesNanjing 210008China

Population growth and growing demand for livestock products produce large amounts of manure,which can be harnessed to maintain soil sustainability and crop ***,the impacts of excessive manure application on crop yields,nitrogen(N)-cycling processes and microorganisms remain ***,we explored the effects of 20-year of excessive rates(18 and 27 Mg ha^(–1)yr^(–1))of pig manure application on peanut crop yields,soil nutrient contents,N-cycling processes and the abundance of N-cycling microorganisms in an acidic Ultisol in summer and winter,compared with none and a regular rate(9 Mg ha^(–1)yr^(–1))of pig manure ***-term excessive pig manure application,especially at the high-rate,significantly increased soil nutrient contents,the abundance of N-cycling functional genes,potential nitrification and denitrification activity,while it had a weaker effect on peanut yield and plant *** with manure application,seasonality had a much weaker effect on N-cycling gene *** forest analysis showed that available phosphorus(AP)content was the primary predictor for N-cycling gene abundance,with significant and positive associations with all tested N-cycling *** study clearly illustrated that excessive manure application would increase N-cycling gene abundance and potential N loss with relatively weak promotion of crop yields,providing significant implications for sustainable agriculture in the acidic Ultisols.

关键词： denitrification manure amendment nitrification N-cycling functional genes peanut yields

Achieving Synergistic Improvement in Dielectric and Energy Storage Properties of All-Organic Poly(Methyl Methacrylate)-Based Copolymers Via Establishing Charge Traps

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Energy & Environmental Materials 2024年第2期7卷 308-319页

作者： Guanghu he Huang Luo Chuanfang Yan Yuting wan Dang Wu Hang Luo Yuan Liu Sheng Chen Key Laboratory of Polymeric Materials and Application Technology of Hunan Province College of ChemistryXiangtan UniversityXiangtan 411105China State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China Guangdong university of Petrochemical Technology Maoming 525000China

How to achieve synergistic improvement of permittivity(ε_(r))and breakdown strength(E_(b))is a huge challenge for polymer ***,for the first time,theπ-conjugated comonomer(MHT)can simultaneously promote theε_(r)and E_(b)of linear poly(methyl methacrylate)(PMMA)*** PMMA-based random copolymer films(P(MMA-co-MHT)),block copolymer films(PMMA-b-PMHT),and PMMA-based blend films were prepared to investigate the effects of sequential structure,phase separation structure,and modification method on dielectric and energy storage properties of PMMA-based dielectric *** a result,the random copolymer P(MMA-coMHT)can achieve a maximumε_(r)of 5.8 at 1 kHz owing to the enhanced orientation polarization and electron *** electron injection and charge transfer are limited by the strong electrostatic attraction ofπ-conjugated benzophenanthrene group analyzed by the density functional theory(DFT),the discharge energy density value of P(MMA-co-PMHT)containing 1 mol%MHT units with the efficiency of 80%reaches15.00 J cm^(-3)at 872 MV m^(-1),which is 165%higher than that of pure *** study provides a simple and effective way to fabricate the high performance of polymer dielectrics via copolymerization with the monomer of P-type semi-conductive polymer.

关键词： dielectric capacitor electrical properties energy density polymer dielectric semiconductor polymer

Synthesis and potential osteogenic applications of Wnt3a-loaded ZIF-8 nanoparticles

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Chinese Chemical Letters 2024年第3期35卷 399-405页

作者： hengfei wang Song Chen Zihan he Junyu Chen Zhou Zhu Qianbing wan Jian wang Xibo Pei State Key Laboratory of Oral Diseases National Clinical Research Center for Oral DiseasesDepartment of ProsthodonticsWest China Hospital of StomatologySichuan UniversityChengdu 610041China chongqing Key Laboratory of Oral Diseases and Biomedical Sciences Chongqing Municipal Key Laboratory of Oral Biomedical Engineering of Higher EducationStomatological Hospital of Chongqing Medical UniversityChongqing 400016China

The Wnt signaling pathway plays a critical role in bone homeostasis,and the related protein therapy strategies have been reported to have great potential in osseointegration;however,they face formidable challenges such as complex external environments and unavoidable protein *** this work,we report a novel approach combining the synthesis of metal–organic frameworks(MOFs)and protein encapsulation in a one-pot process based on zeolitic imidazolate framework-8(ZIF-8)and Wnt3a protein,with improved biomechanical behavior and enhanced protein biological *** combination was designed to enhance the Wnt3a protein function through the improved chemical stability provided by the ZIF-8 ***,the zinc ions contained in the ZIF-8 crystals induced bone homeostasis,further favoring the *** results showed that the Wnt3a protein-loaded ZIF-8 crystals served as efficient drug delivery vehicles to promote osteogenesis,preventing protein *** particular,Wnt3a-loaded ZIF-8 nanoparticles(Wnt3a@ZIF-8 NPs)had higher efficacy on bone marrow mesenchymal stem cells(BMSCs)than ZIF-8 NPs or Wnt3a proteins,contributing to the osteogenesis through ZIF-8 crystals and intracellular Wnt3a proteins released from Wnt3a@ZIF-8 ***,polymerase chain reaction(PCR)analysis showed that the osteogenic pathways were ***,the present one-pot process can open up new avenues to develop signaling protein-delivery systems for applications in protein therapy strategies.

关键词： Metal–organic frameworks Nanoparticle Drug release Osteogenesis Bone defects

Whispering-gallery-mode barcode-based broadband sub-femtometer-resolution spectroscopy with an electro-optic frequency comb

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Advanced Photonics 2024年第1期6卷 115-125页

作者： Bingxin Xu Yangyang wan Xinyu Fan Zuyuan he Shanghai Jiao Tong university State Key Laboratory of Advanced Optical Communication Systems and NetworksDepartment of Electronic EngineeringShanghaiChina Max-Planck Institute of Quantum Optics Hans-Kopfermann-Straûe 185748 GarchingGermany

Spectroscopy is the basic tool for studying molecular physics and realizing biochemical ***,it is challenging to realize sub-femtometer resolution spectroscopy over broad *** and high-resolution spectroscopy with calibrated optical frequency is demonstrated by bridging the fields of speckle pattern and electro-optic frequency comb.A wavemeter based on a whispering-gallery-mode barcode is proposed to link the frequencies of a probe continuous-wave laser and an ultrastable *** ultrafine electro-optic comb lines are generated from the probe laser to record spectrum of sample with sub-femtometer *** bandwidth is a thousandfold broader than comb bandwidth,by sequentially tuning the probe laser while its wavelength is *** approach fully exploits the advantages of two fields to realize 0.8-fm resolution with a fiber laser and 80-nm bandwidth with an external cavity diode *** spectroscopic measurements of an ultrahigh Q-factor cavity and gas molecular absorption are experimentally *** compact system,predominantly constituted by few-gigahertz electronics and telecommunication components,shows enormous potential for practical spectroscopic applications.

关键词： frequency comb reconstructive wavemeter spectroscopy

Functional divergences of natural variations of TaNAM-A1 in controlling leaf senescence during wheat grain filling

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Journal of Integrative Plant Biology 2024年第6期66卷 1242-1260页

作者： Longxi Zhou Guowei Chang Chuncai Shen wan Teng Xue he Xueqiang Zhao Yanfu Jing Zhixiong Huang Yiping Tong Key Laboratory of Seed Innovation Institute of Genetics and Developmental SciencesChinese Academy of SciencesBeijing 100101China university of Chinese Academy of Sciences Beijing 100049China The Innovative Academy of Seed Design Chinese Academy of SciencesBeijing 100101China

Leaf senescence is an essential physiological process related to grain yield potential and nutritional *** leaf duration(GLD)after anthesis directly reflects the leaf senescence process and exhibits large genotypic differences in common wheat;however,the underlying gene regulatory mechanism is still ***,we identified TaNAM-A1 as the causal gene of the major loci q GLD-6A for GLD during grain filling by map-based *** assays and TILLING mutant analyses demonstrated that TaNAM-A1 played a critical role in regulating leaf senescence,and also affected spike length and grain ***,the functional divergences among the three haplotypes of TaNAM-A1 were systematically *** varieties with TaNAM-A1d(containing two mutations in the coding DNA sequence of TaNAM-A1)exhibited a longer GLD and superior yield-related traits compared to those with the wild type *** three haplotypes were functional in activating the expression of genes involved in macromolecule degradation and mineral nutrient remobilization,with TaNAM-A1a showing the strongest activity and TaNAM-A1d the ***-A1 also modulated the expression of the senescencerelated transcription factors TaNAC-S-7A and ***016-3A enhanced the transcriptional activation ability of TaNAM-A1a by protein–protein interaction,thereby promoting the senescence *** study offers new insights into the fine-tuning of the leaf functional period and grain yield formation for wheat breeding under various geographical climatic conditions.

关键词： allelic variation leaf senescence map-based cloning TaNAM-A1 transcription factor Triticum aestivum

Hyphae-mediated bioassembly of carbon fibers derivatives for advanced battery energy storage

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Carbon Energy 2024年第6期6卷 140-150页

作者： Lei Huang Zhong Qiu Ping Liu Xinhui Xia Feng Cao Xinping he Chen wang wangjun wan Yongqi Zhang Yang Xia Wenkui Zhang Minghua Chen Jiancang Zhou Department of Critical Care Medicine Sir Run Run Shaw HospitalSchool of MedicineZhejiang UniversityHangzhouChina State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang ProvinceSchool of Materials Science&EngineeringZhejiang UniversityHangzhouChina College of Materials Science&Engineering Zhejiang University of TechnologyHangzhouChina State Key Laboratory of Photocatalysis on Energy and Environment Fuzhou UniversityFuzhouChina Department of Engineering Technology Huzhou CollegeHuzhouChina Zhejiang Academy of Science and Technology for Inspection&Quarantine HangzhouZhejiangChina Institute of Fundamental and Frontier Science University of Electronic Science and Technology of ChinaChengduChina Key Laboratory of Engineering Dielectric and Applications(Ministry of Education) School of Electrical and Electronic EngineeringHarbin University of Science and TechnologyHarbinChina

Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power ***,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite *** mechanism of biological adsorption assembly is also *** a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur *** this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are ***,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium ***,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.

关键词： bioassembly carbon fibers energy storage graphene lithium-sulfur batteries

A case study of comparing two dimerized acceptor molecules built by different branch-connected and terminal-connected approaches

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Science china Chemistry 2024年第5期67卷 1687-1696页

作者： Kangqiao Ma Huazhe Liang Yuxin wang Tengfei he Tainan Duan Xiaodong Si Wendi Shi Guankui Long Xiangjian Cao Zhaoyang Yao Xiangjian wan Chenxi Li Bin Kan Yongsheng Chen State Key Laboratory and Institute of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsInstitute of Polymer ChemistryRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials Science and Engineering National Institute for Advanced MaterialsRenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300350China chongqing Institute of Green and Intelligent Technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400015China

Dimerized small-molecule acceptors(SMAs) built by the conventional connection of terminal groups of monomers have contributed to exciting long-term stabilities of organic solar cells(OSCs). However, device efficiencies, especially fill factors(FFs), still need to be improved. This probably originates from unsymmetrical molecular structure/conformation-determined less compact/ordered molecular stackings, such as ineffective stackings of constraint terminals. herein, an exotic dimerized SMA of BC-Th is established by bridging the branched groups(BC-type, branch coupling) of two monomers rather than conventional terminal units(TC-type, terminal coupling). Benefiting from the three-dimensional conformation and more uncurbed terminals,BC-Th exhibits multiple molecular orientations along with a larger dielectric constant and electron mobility compared with TCTh. Finally, an efficiency of 17.43% is achieved by BC-Th-based OSCs, along with the highest FF of 79.13% among all dimerized SMAs-based OSCs to date. When introducing L8-BO as the third component, overall enhanced efficiency of 18.05%and FF of 80.11% are further afforded. Contrarily, TC-Th-based OSCs exhibit much inferior PCE of 16.29% and FF of 74.81%,demonstrating the great advantages of “branch coupling” over “terminal coupling” when building dimerized SMAs.

关键词： organic solar cells dimerized acceptor molecules branch coupling morphology control stability