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Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe12]16+ Core

National science Review 2024年第4期11卷 123-129页

作者： Gan Xu Yun-Shu Cui Xue-Lian Jiang Cong-Qiao Xu Jun Li Xu-Dong Chen Jiangsu Collaborative Innovation Center of Biomedical Functional Materials and Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua University State Key Laboratory of Coordination Chemistry Nanjing University

Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage ***,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron *** this work,we have synthesized,crystallized,and characterized a（Tp*）4W4S12(Fe@Fe12) cluster(Tp*=tris（3,5-dimethyl-1-pyrazolyl）borate（1-）),which features a rare trideca-nuclear,icosahedral[Fe@Fe12] cluster core with direct multicenter iron-iron bonding between the interstitial iron（Fei） and peripheral irons（Fep）,as well as Fep…Fepferromagnetic *** chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the [Fe@Fe12]16+core,assisted by its bonding interactions with the peripheral tridentate [（Tp*）WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-Wσ *** ground-state electron spin is theoretically predicted to be S=32/2 for the *** existence of low oxidation-state（OS～+1.23） iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.

关键词： Fe13 cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

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Identifying and Engineering Active Sites at the Surface of Porous Single-Crystalline Oxide Monoliths to Enhance Catalytic Activity and Stability

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CCS Chemistry 2022年第4期4卷 1441-1451页

作者： Guoming Lin Hao Li Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108 Advanced Energy Science and Technology Guangdong Laboratory HuizhouGuangdong 116023

Identifying and engineering active sites play a key role in many catalytic ***,we create well-defined surface structures through the growth of porous single-crystalline Mn_(3)O_(4) and Mn_(2)O_(3) monoliths at centimeter scale and confine atomically dispersed Pt ions in the lattice at the twisted surface to construct isolated active *** activation of lattice oxygen linked to isolated Pt ions is much more effective than the lattice oxygen linked to Mn ions in local structures,leading to an approximately sevento eightfold enhancement of surface oxygen exchange coefficients for catalytic CO *** active structures of PtO_(1.5) and PtO_(1.4) confined at the well-defined surfaces contribute to the efficient activation of lattice oxygen linked to Pt ions in local structures in addition to the chemisorption of CO in the oxidation *** demonstrate the complete CO oxidation with air at 65℃ without degradation being observed even after continuous operation of 300 h.

关键词： porous single crystal active site lattice oxygen activation stability

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Agarose hydrogel doped with soluble Se-chitosan for Se-enriched cultivation of sprouts

Advanced Agrochem

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advanced Agrochem 2023年第4期2卷 356-363页

作者： Yun Wang Wei Yang Jian Zhu Qifei Chen Na Li Suzhou Key Laboratory of Green Chemical Engineering School of Chemical and Environmental EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China Faculty of Food Science and Technology Suzhou Polytechnic Institute of AgricultureSuzhou215008China Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationDepartment of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China China Shenhua Coal to Liquid and Chemical Co.Ltd. Beijing100011China

Se-chitosan with a high Se content of 139 mg/g was successfully synthesized using the glacial acetic acid-sodium selenite(HAc-Na2SeO3)*** chemical structure of Se-chitosan was characterized by FTIR,XRD,TGA,UV–vis and 13C NMR,confirming that selenite acid was introduced into chitosan via the esterification reaction of the hydroxyl group at C6 and the electrostatic interaction of the amino group at C2 of *** hydrogels were designed as an efficient carrier of Se-chitosan for Se-enriched cultivation of *** hydrogels exhibited a porous structure,which is beneficial for Se diffusion in *** growth indexes of sprouts grown in Agar/Se-chitosan composite hydrogels with different Se concentrations,including plant weight,plant height and Se content,were *** results showed that in the Se-enriched cultivation of sprouts,Se-chitosan possessed an excellent Se enrichment *** the Se concentration in Agar/Se-chitosan composite hydrogels increases from 0 to 1600μg/L,the Se content of the sprouts will also increase from 0.92 mg/kg to 6.79 mg/kg ***,it is necessary to control the amount of Se-chitosan added to the hydrogels;otherwise,the growth of sprouts will be *** research provided a simple and effective method for the fabrication of Secontaining hydrogels for Se-enriched cultivation of sprouts.

关键词： Hydrogel Se-chitosan Agarose hydrogel Sprouts Se enrichment

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In situ preparation of gel polymer electrolyte for lithium batteries: Progress and perspectives

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InfoMat 2022年第2期4卷 110-125页

作者： Chao Ma Wenfeng Cui Xizheng Liu Yi Ding Yonggang Wang Tianjin Key Laboratory of Advanced Functional Porous Materials Institute for New Energy Materials and Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjinChina Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghaiChina

The practical applications of Li-ion batteries(LIBs)are challenged by their safety concerns when using liquid electrolytes(LEs).Solid-state gel polymer electrolytes(GPEs)can address this challenge and have drawn increased attention ***,GPEs are prepared separately and then assembled into cells,which undoubtedly result in dissatisfactory solid/solid interfacial compatibility and low ionic ***,in situ GPEs are proposed to address the above challenges and simplify the preparation ***,LE precursor is injected into the cells and gradually transformed into a quasisolid gel state under the conditions of thermal or chemical ***,the obtained in situ GPEs could fully infiltrate the electrode and better interface contact of gel electrolyte/electrode is thus *** this review,the authors focus on the in situ GPEs used in lithium batteries(LBs),and summarize recent progress of the design,synthesis,and applications of in situ *** on the different ways of triggering polymerization,there are mainly three methods:thermochemical gelation,polymerization by additional chemical initiators,and cross-linking initiated by Li O *** GPEs based on in situ solidification method are introduced as a promising strategy to improve the electrochemical ***,up-to-date research progresses are discussed,and perspectives are provided on the development and challenges of in situ GPEs to meet the requirements for their practical applications in LBs.

关键词： cross-linking gel electrolytes in situ preparation Li-metal batteries polymerization

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Phase Engineering of CoMo0_(4)Anode Materials toward Improved Cycle Life for Li^(+)Storage

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Chinese Journal of Chemistry 2021年第5期39卷 1121-1128页

作者： Xiaoqing Huang Junhao Li Wenbiao Zhang Wenjie Huang Lichun Yang Qingsheng Gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhouGuangdong 510632China School of Materials Science and Engineering and Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhouGuangdong 510641China

Anode materials based on conversion reactions usually possess high energy densities for lithium-ion batteries(LIBs).However,they suffer from poor rate performance and cycle life due to serious volume ***,α/β-CoMo04 heterogeneous nanorods are synthesized via a facile co-precipitation method,and further are phase-engineered through varying calcination temperature,accomplishing the obviously improved cycle life and rate performance as anodes for *** evaluated at a current density of 1.0 A·g^(-1)the optimal nanorods with anα/βphase ratio of 6.0 afford the reversible capacity of 1143.6 mAh·g^(-1)after 200 cycles,outperforming most of recently reported bimetal ***^(+)storage mechanism is further analyzed by using in-situ X-ray diffraction and ex-situ transition electronic ***'s revealed thatβ-CoMoO_(4)follows a one-step conversion reaction;whileα-CoMo0_(4)proceeds an intercalation pathway before the conversion *** storage of Li^(+)would alleviate the volume effect of heterostructuredα/β-CoMo0_(4),forming electronically conductive network evenly composed of Co and Mo nanograins to enable the reversible electrochemical *** work is anticipated to give some hints for the rational design of high-performance energy materials.

关键词： Electrochemistry Anode materials Bimetal oxides Crystal engineering Reaction mechanisms

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Sodium-Ion Battery Anode Construction with SnP_(x)Crystal Domain in Amorphous Phosphorus Matrix

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Energy Material Advances 2021年第1期2021卷 37-47页

作者： Baixu Chen Yubo Yang Aibing Chen Xu Zhang Jaffer Saddique Mingxue Tang Haijun Yu Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China College of Materials Science&Technology Jiangsu Key Laboratory of Materials and Technology for Energy ConversionNanjing University of Aeronautics&AstronauticsNanjing 210016China Center for High Pressure Science&Technology Advanced Research Beijing 100094China

The high-capacity phosphorus-(P-)based anode materials for sodium-ion batteries(NIBs)often face poor performance retentions owing to the low conductivity and large volume *** is thus essential to buffer these problems by appropriately alloying with other elements such as tin(Sn)and constructing well-designed ***,a series of P-/Sn-based composites have been synthesized by the facile and low-cost one-step ball *** distribution function(PDF)has been employed as a hardcore quantitative technique to elucidate their structures combined with other techniques,suggesting the formation and ratios of Sn4P3 and Sn crystalline domains embedded inside an amorphous P/carbon *** composite with the largest amount of Sn4P3 in the P/C matrix can deliver the most balanced electrochemical performance,with a capacity of 422.3 mA-h g^(−1 )for 300 cycles at a current density of 1000mAg^(−1).The reaction mechanism has been elucidated by 23Na and 31P solid-state nuclear magnetic resonance(NMR)*** study sheds light on the rational design and concrete identification of P-/Sn-based amorphous-dominant composite materials for NIBs.

关键词： alloying amorphous composite

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Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

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Nano Research 2021年第4期14卷 998-1003页

作者： Wenjie Wu Yan Liu Dong Liu Wenxing Chen Zhaoyi Song Ximin Wang Yamin Zheng Ning Lu Chunxia Wang Junjie Mao Yadong Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of PetroleumBeijing 102249China Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based MaterialsAnhui Normal UniversityWuhu 241002China State key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively ***,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu_(1)/NC)was prepared by coordination pyrolysis ***,the Cu_(1)/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(***)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol ***,the Cu_(1)/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/*** experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu_(1)/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR *** study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.

关键词： single atomic sites catalysts nitrogen-doped carbon materials oxygen reduction reaction carbon defect non-noble metal

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In Situ Iodide Passivation Toward Efficient CsPbI_(3) Perovskite Quantum Dot Solar Cells

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Nano-Micro Letters 2023年第10期15卷 28-39页

作者： Junwei Shi Ben Cohen‑Kleinstein Xuliang Zhang Chenyu Zhao Yong Zhang Xufeng Ling Junjun Guo Doo‑Hyun Ko Baomin Xu Jianyu Yuan Wanli Ma Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055People’s Republic of China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow University199 Ren‑Ai RoadSuzhou Industrial ParkSuzhou 215123People’s Republic of China Department of Electrical and Computer Engineering University of British Columbia2329 West MallVancouverBC V6T 1Z4Canada Department of Chemistry Sungkyunkwan UniversitySuwon 16419Republic of Korea Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University199 Ren‑Ai RoadSuzhou Industrial ParkSuzhou 215123People’s Republic of China Jiangsu Key Laboratory for Carbon‑Based Functional Materials&Devices Soochow University199 Ren‑Ai RoadSuzhou Industrial ParkSuzhou 215123People’s Republic of China

All-inorganic CsPbI_3 quantum dots(QDs) have demonstrated promising potential in photovoltaic(PV) applications. However, these colloidal perovskites are vulnerable to the deterioration of surface trap states, leading to a degradation in efficiency and stability. To address these issues, a facile yet effective strategy of introducing hydroiodic acid(HI) into the synthesis procedure is established to achieve high-quality QDs and devices. Through an in-depth experimental analysis, the introduction of HI was found to convert PbI_2 into highly coordinated [PbI_m]~(2-m), enabling control of the nucleation numbers and growth kinetics. Combined optical and structural investigations illustrate that such a synthesis technique is beneficial for achieving enhanced crystallinity and a reduced density of crystallographic defects. Finally, the effect of HI is further reflected on the PV performance. The optimal device demonstrated a significantly improved power conversion efficiency of 15.72% along with enhanced storage stability. This technique illuminates a novel and simple methodology to regulate the formed species during synthesis, shedding light on ofurther understanding solar cell performance, and aiding the design of future novel synthesis protocols for high-performance optoelectronic devices.

关键词： CsPbI_(3)perovskite quantum dots In situ passivation Surface trap states Perovskite solar cell

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Hornbill: A Portable, Touchless, and Battery-Free Electrochemical Bio-tag for Multi-pesticide Detection 24

Hornbill: A Portable, Touchless, and Battery-Free Electroche...

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30th International Conference on Mobile Computing and Networking, ACM MobiCom 2024

作者： He, Guorong Xie, Yaxiong Zheng, Chao Zhang, Longlong Wu, Qi Zhang, Wenyan Xu, Dan Chen, Xiaojiang Northwest University Xi'an China University at Buffalo SUNY New York United States Shaanxi International Joint Research Centre for the Battery-Free Internet of Things China Xi'an Advanced Battery-Free Sensing and Computing Technology International Science and Technology Cooperation Base China Internet of Things Research Center Northwest University China Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education China

ISBN: (纸本)9798400704895

Pesticide overuse poses significant risks to human health and environmental integrity. Addressing the limitations of existing approaches, which struggle with the diversity of pesticide compounds, portability issues, and environmental sensitivity, this paper introduces Hornbill. A wireless and battery-free electrochemical bio-tag that integrates the advantages of NFC technology with electrochemical biosensors for portable, precise, and touchless multi-pesticide detection. The basic idea of Hornbill is comparing the distinct electrochemical responses between a pair of biological receptors and different pesticides to construct a unique set of feature fingerprints to make multi-pesticide sensing feasible. To incorporate this idea within small NFC tags, we reengineer the electrochemical sensor, spanning the antenna to the voltage regulator. Additionally, to improve the system's sensitivity and environmental robustness, we carefully design the electrodes by combining microelectrode technology and materials science. Experiments with 9 different pesticides show that Hornbill achieves a mean accuracy of 93% in different concentration environments and its sensitivity and robustness surpass that of commercial electrochemical sensors. © 2024 Copyright is held by the owner/author(s). Publication rights licensed to ACM.

关键词： Electrochemical biosensors

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Low-lying electronic states with giant linear dichroic ratio observed in PdSe2

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Physical Review B 2022年第12期106卷 L121110-L121110页

作者： Chenyi Gu Xiaowei Liu Cheng Chen Aiji Liang Wei Guo Xinrui Yang Jian Zhou Chris Jozwiak Aaron Bostwick Zhongkai Liu Shi-Jun Liang Yulin Chen Feng Miao Eli Rotenberg Yuefeng Nie National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials College of Engineering and Applied Sciences Nanjing University Nanjing 210093 China Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China Institute of Brain-Inspired Intelligence National Laboratory of Solid State Microstructures School of Physics Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China School of Physical Science and Technology ShanghaiTech University Shanghai 201210 China ShanghaiTech Laboratory for Topological Physics Shanghai 201210 China Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Department of Physics University of Oxford Oxford OX1 3PU United Kingdom

Palladium diselenide (PdSe2), a recently exploited transition metal dichalcogenide material with a thickness-dependent band gap, anisotropic optical response, and high air stability, has shown excellent performance in electronics and polarization photodetection. However, the origin of the intriguing optical response in this material from a perspective of electronic band structure, including the orbital character and the experimental demonstration of its indirect band gap, has not yet been explored. By applying polarization-dependent, angle-resolved photoemission spectroscopy and density functional theory calculations, we measured an indirect band gap of bulk PdSe2 to be ∼0.36eV. Moreover, the orbital-resolved electronic band structure reveals a top valence band dominated by Pd-d3z2−r2 and Se-pz orbitals, which gives rise to an unprecedented giant linear dichroic ratio of 10, showing a huge orbital-induced anisotropy. Our results elucidate the semiconducting nature of PdSe2 and propose PdSe2 to be an intrinsically orbital-engineered material with giant anisotropy for polarization-related optical applications.

关键词： Band gap Density functional theory Electronic structure Layered semiconductors Polarization Angle-resolved photoemission spectroscopy

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