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Engineering egOrbital Occupancy of Pt with Au Alloying Enables Reversible Li−O2Batteries

Angewandte Chemie 2022年第26期134卷

作者： Yin Zhou Qianfeng Gu Kun Yin Yiju Li Lu Tao Hao Tan Yong Yang Prof. Shaojun Guo School of Materials Science and Engineering Peking University Beijing 100871 China Department of Materials Science and Engineering City University of Hong Kong Tat Chee Avenue 83 Kowloon Hong Kong 999077 China Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications School of Materials Science & Engineering Beijing Institute of Technology Beijing 10081 China State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal Materials Northwestern Polytechnical University Xi'an 710072 China

Constructing well-designed catalysts to accelerate OER catalytic activity and alleviate the charge overpotential is prevailing for achieving sophisticated Li−O 2 batteries. Herein, we report a concept for engineering the e g occupancy of Pt with M alloying (M=Au, Ru) to tune the charge overpotentials for achieving high-performance Li−O 2 batteries. The X-ray photoelectron spectroscopy results coupled with density functional theory (DFT) calculations reveal that the highly electronegative Au can capture more e g electrons from Pt, leading to less e g electrons of Pt in PtAu than that in PtRu. The lower e g occupancy of Pt atoms in PtAu alloys entails the upward shift of the Pt d band, which causes a strong binding strength towards the intermediates (LiO 2 ), thereby decreasing the OER energy barrier. As a consequence, the Li−O 2 battery with a PtAu cathode delivers a low charge overpotential of 0.36 V and superior cycle life of 220 cycles at a cutoff capacity of 1000 mAh g −1 , which is among the best in the reported noble metal-based cathodes.

关键词： Adsorption Strength Antibonding Orbital eg Occupancy Li−O2 Batter PtAu Nanocrystals

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Dimensional control of octahedral tilt in SrRuO3 via infinite-layered oxides

arXiv

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arXiv 2021年

作者： Lin, Shan Zhang, Qinghua Sang, Xiahan Zhao, Jiali Cheng, Sheng Huon, Amanda Jin, Qiao Chen, Shuang Chen, Shengru Guo, Haizhong He, Meng Ge, Chen Wang, Can Wang, Jia-Ou Fitzsimmons, Michael R. Gu, Lin Zhu, Tao Jin, Kui-Juan Guo, Er-Jia Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing100049 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research Center Wuhan University of Technology 122 Luoshi Rd. Wuhan430070 China Institute of High Energy Physics Chinese Academy of Sciences Beijing100049 China Spallation Neutron Source Science Center Dongguan523803 China School of Physical Sciences University of Chinese Academy of Sciences Beijing100190 China Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37831 United States School of Physical Engineering Zhengzhou University Zhengzhou450001 China Songshan Lake Materials Laboratory DongguanGuangdong523808 China

Manipulation of octahedral distortion at atomic length scale is an effective means to tune the physical ground states of functional oxides. Previous work demonstrates that epitaxial strain and film thickness are variable parameters to modify the octahedral rotation and tilt. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetic response in SrRuO3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO2 (SCO) layers. The infinite-layered CuO2 in SCO exhibits a structural transformation from "planar-type" to "chain-type" as reducing film thickness. These two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and hybridization strength between Ru 4d and O 2p orbitals, leading to a significant change in the magnetoresistance and anomalous Hall resistivity of SRO layers. These findings could launch further investigations into adaptive control of magnetoelectric properties in quantum oxide heterostructures using oxygen coordination. © 2021, CC BY.

关键词： Ruthenium compounds

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Engineering Bi 2 WO 6 -loaded TiO 2 nanotubes for enhanced photocatalytic organic wastewater degradation and photoelectric conversion

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Environmental Research 2025年 282卷

作者： Xinming Guo Junjie Zhang Juntong Xu Xiangsheng Dan Fuqiang Guo Baohua Zhang Lili Zhang Qingyao Wang Junwei Hou Xinjiang Key Laboratory of Phase Transitions and Microstructures in Condensed Matters College of Physical Science and Technology Yili Normal University Yining 835000 China Xinjiang Key Laboratory of High Value Green Utilization of Low-rank Coal School of Physics and Materials Science Changji University Changji 831100 China Anhui Engineering Research Center for High Efficiency Intelligent Photovoltaic Module Chaohu University Hefei 238000 China State Key Laboratory of Heavy Oil Processing China University of Petroleum (Beijing) at Karamay Karamay 834000 China

The adjustment of the microstructure and morphology of catalysts is highly significant for enhancing photocatalytic performance, which is particularly important because the morphology and interfacial properties of composite photocatalysts play a crucial role in charge carrier transportation and overall photocatalytic activity. In this paper, TiO 2 nanotube arrays/Bi 2 WO 6 (TiO 2 NTs/Bi 2 WO 6 ) photocatalysts with excellent heterojunction interfaces were synthesized using the one-step solvothermal method by varying the type of solvent. The hierarchical morphology effectively improved the catalyst's light absorption capacity and electron transportation ability, demonstrating excellent performance in the photoelectric conversion and degradation of organic pollutants. The research results indicated that the TiO 2 NTs/Bi 2 WO 6 photocatalysts exhibited outstanding performance in the degradation of crystal violet (CV), tetracycline (TC), and methylene blue (MB) dyes, achieving degradation efficiencies of 95.63 %, 62.34 % and 98.29 %, respectively, while also showing strong stability, maintaining high photocatalytic activity even after multiple cycles. Furthermore, this investigation revealed the influencing factors and active groups in the photocatalytic degradation of dyes and proposed the mechanism for the photocatalytic degradation of organic dye wastewater. This study also tested the intermediate products and the toxicity in the photocatalytic degradation of TC, and proposed three potential degradation pathways. The investigation on the impact of solvent type on catalyst synthesis and activity performance provides valuable insights and guidance for the synthesis of photocatalysts and the treatment of organic wastewater.

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Quantum metric nonlinear spin-orbit torque enhanced by topological bands

Materials Today Quantum

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materials Today Quantum 2025年 6卷

作者： Xukun Feng Weikang Wu Hui Wang Weibo Gao Lay Kee Ang Y.X. Zhao Cong Xiao Shengyuan A. Yang Science Mathematics and Technology Cluster Singapore University of Technology and Design Singapore 487372 Singapore Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials (Ministry of Education) Shandong University Jinan 250061 China Shandong Key Laboratory of Advanced Structural Materials Genome Engineering Shandong University Jinan 250061 China Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore 637371 Singapore Department of Physics The University of Hong Kong Hong Kong China Interdisciplinary Center for Theoretical Physics and Information Sciences (ICTPIS) Fudan University Shanghai 200433 China Research Laboratory for Quantum Materials IAPME FST University of Macau Macao Special Administrative Region of China

Effects manifesting quantum geometry have been a focus of physics research. Here, we reveal that quantum metric plays a crucial role in nonlinear electric spin response, leading to a quantum metric spin–orbit torque. We argue that enhanced quantum metric can occur at band (anti)crossings, so the nonlinear torque could be amplified in topological metals with nodal features close to Fermi level. By applying our theory to magnetic Kane–Mele model and monolayer CrSBr, which feature nodal lines and Weyl points, we demonstrate that the quantum metric torque dominates the response, and its magnitude is significantly enhanced by topological band structures, which even surpasses the previously reported linear torques and is sufficient to drive magnetic switching by itself.

关键词： First-principles calculations Spintronics Spin generation Transport phenomena

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Waste biomass-assisted synthesis of TiO 2 and N/O-contained graphene-like biochar composites for enhanced adsorptive and photocatalytic performances

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Journal of Alloys and Compounds 2022年 899卷

作者： Hao Luo Shunli Yu Ming Zhong Yuqi Han Bitao Su Ziqiang Lei Key Laboratory of Eco-Functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-Environmental Polymer Materials of Gansu Province College of Chemistry and Chemical Engineering Northwest Normal University Lanzhou 730070 PR China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of Technology Lanzhou 730050 PR China College of Chemistry and Chemical Engineering He Xi University Zhangye 734000 PR China

Titanium dioxide (TiO 2 ) is a promising semiconductor photocatalyst for degradation of organic pollutants but is hampered by bandwidth prohibition and high probability of photo-generated electron-hole recombination. Searching for effective modification strategies to alleviate these issues is thus particularly significant. Herein, two series of composites of TiO 2 and graphene-like biochar (PC) were prepared via a simple biomass-assisted pyrolysis coupled with activation strategy and characterized by various techniques. The methylene blue (MB)-simulated waste water was used to evaluate their adsorptive and photocatalytic performances. The results showed that the optimal TiO 2 -PC composite delivered an excellent photocatalytic performance, nearly 4 times as TiO 2 . The enhanced performance was probably caused by the synergistic effect among the graphene-like PC, the self-introduced N/O heteroatom, and the interaction between TiO 2 and PC. Furthermore, the possible photocatalytic process was also proposed. This work may provide a guidance on preparing high-performance composites through a simple, cheap, and environmental biomass-assisted strategy for highly-efficient photocatalysis application.

关键词： Biomass TiO 2 Biochar Characterization Adsorptive and photocatalytic performances

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Carbon–carbon bond cleavage for a lignin refinery

Nature Chemical Engineering

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Nature Chemical Engineering 2024年第1期1卷 61-72页

作者： Zhicheng Luo Alexandra Radu Davey F. de Waard Panos D. Kouris Michael D. Boot Emiel J. M. Hensen Yun Wang Jun Xiao Huiyan Zhang Rui Xiao Chong Liu Jean T. Behaghel de Bueren Jeremy S. Luterbacher Laboratory of Inorganic Materials and Catalysis Department of Chemical Engineering and Chemistry Eindhoven University of Technology Eindhoven the Netherlands MOE Key Laboratory of Energy Thermal Conversion & Control School of Energy and Environment Southeast University Nanjing China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian China Laboratory of Sustainable and Catalytic Processing Institute of Chemical Sciences and Engineering Ecole Polytechnique Fédérale de Lausanne Lausanne Switzerland

Carbon–carbon bonds, ubiquitous in lignin, limit monomer yields from current depolymerization strategies, which mainly target C–O bonds. Selective cleavage of the inherently inert σ-type C–C bonds without pre-functionalization remains challenging. Here we report the breaking of C–C bonds in lignin obtained upon initial disruption of labile C–O bonds, achieving monocyclic hydrocarbon yields up to an order of magnitude higher than previously reported. The use of a Pt (de)hydrogenation function leads to olefinic groups close to recalcitrant C–C bonds, which can undergo β-scission over zeolitic Brønsted acid sites. After confirming that this approach can selectively cleave common C–C linkages (5–5′, β–1′, β–5′ and β–β′) in lignin skeletons, we demonstrate its utility in the valorization of various representative lignins. A techno-economic analysis shows the promise of our method for producing gasoline- and jet-range cycloalkanes and aromatics, while a life-cycle assessment confirms its potential for CO2-neutral fuel production.

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Highly Textured N-Type SnSe Polycrystals with Enhanced Thermoelectric Performance

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研究（英文） 2020年第2期 267-276页

作者： Peng-Peng Shang Jinfeng Dong Jun Pei Fu-Hua Sun Yu Pan Huaichao Tang Bo-Ping Zhang Li-Dong Zhao Jing-Feng Li State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua UniversityBeijing 100084 China College of Chemistry and Material Science Shandong Agricultural University Tai'an 271018 China The Beijing Municipal Key Laboratory of New Energy Materials and Technologies School of Materials Science and EngineeringUniversity of Science and Technology Beijing Beijing 100083 China School of Materials Science and Engineering Beihang University Beijing 100191 China

Thermoelectric materials,which directly convert heat into electricity based on the Seebeck effects,have long been investigated for use in semiconductor refrigeration or waste heat *** them,SnSe has attracted significant attention due to its promising performance in both p-type and n-type crystals;in particular,a higher out-of-plane ZT value could be achieved in n-type SnSe due to its 3D charge and 2D phonon *** this work,the thermoelectric transport properties of n-type polycrystalline SnSe were investigated with an emphasis on the out-of-plane transport through producing textural *** textures were fabricated using mechanical alloying and repeated spark plasma sintering (SPS),as a kind of hot pressing,aimed at producing strong anisotropic transports in n-type polycrystalline SnSe as that in crystalline *** show that the lowest thermal conductivity of 0.36Wm-1 K1 was obtained at 783K in perpendicular to texture ***,the electrical transport properties are less anisotropic and even nearly isotropic,and the power factors reach 681.3μWm-1 K-2 at 783 K along both parallel and perpendicular *** combination of large isotropic power factor and low anisotropic thermal conductivity leads to a maximum ZT of 1.5 at 783 *** high performance elucidates the outstanding electrical and thermal transport behaviors in n-type polycrystalline SnSe,and a higher thermoelectric performance can be expected with future optimizing texture in n-type polycrystalline SnSe.

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Effects of alloy elements on ductility and thermal conductivity of compacted graphite iron

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China Foundry 2018年第3期15卷 189-195页

作者： Dong-mei Xu Gui-quan Wang Xiang Chen Yan-xiang Li Yuan Liu Hua-wei Zhang School of Materials Science and Engineering Tsinghua University Beijing 100084 China Key Laboratory for Advanced Materials Processing Technology (MOE) Tsinghua University Beijing 100084 China

The infl uence of Si, Sn, Mo and Ni on the ductility and thermal conductivity of compacted graphite iron(CGI) was investigated. Metallographic observation and Differential Scanning Calorimetry(DSC) experiments were carried out to analyze the roles of various additions in the eutectoid reaction. The experimental results showed that the ductility of CGI is proportional to the ferrite fraction, so moderate Si content could dramatically improve the ductility by increasing the ferrite fraction. DSC measurements showed that Mo has moderate inhibition on eutectoid transformation during both the heating and cooling processes, while the sample without Sn obviously broadens the three-phase region. Vermicularity and ferrite are known to improve thermal conductivity, and the former plays a more important role. Besides, among the alloy elements investigated, Sn has the greatest negative effect on conductivity, followed by Ni and Mo having the smallest effects.

关键词： compacted graphite iron ductility thermal conductivity

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Fabrication of large-bulk ultrafine grained 6061 aluminum alloy by rolling and low-heat-input friction stir welding

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Journal of materials Science & technology 2018年第1期34卷 112-118页

作者： C.Y.Liu B.Qu P.Xue Z.Y.Ma K.Luo M.Z.Ma R.P.Liu Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Key Laboratory of New Processing Technology for Nonferrous Metal & Materials Ministry of Education Guilin University of Technology Guangxi Key Laboratory of Universities for Clean Metallurgy and Comprehensive Utilization of Nonferrous Metal Resources Guilin University of Technology State Key Laboratory of Metastable Materials Science and Technology Yanshan University

In this study, the ultrafine grained （UFG） 6061 Al alloys fabricated by cold rolling were friction stir welded （FSW） with different rotation rates under both air cooling and rapid cooling in water. Low-heat-input parameters of 400 rpm rotation rate in water （400-Water） could effectively inhibit the coarsening of recrystallized grains, reduce the precipitation rate, and retain more dislocations of the UFG 6061 Al parent metal. 400-Water joint showed high lowest-hardness value, narrow low-hardness zone, and high tensile strength, attributing to the effect of dislocation, grain boundary, solid-solution, and precipitation hardening. This work provides an effective strategy to fabricate large-sized bulk UFG AI alloy by cold rolling with large deformation and low-heat-input FSW.

关键词： Aluminum alloys Ultrafine grained materia Friction stir welding Mechanical properties

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Green synthetic PPy/MXene-based cotton fabric hydrovolt generators for self-powered wearables

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International Journal of Biological Macromolecules 2025年 311卷 143651页

作者： Zhang, Xiaoyang Zhang, Xuefei Ren, Hai-Tao Li, Ting-Ting Lou, Ching-Wen School of Textile Science and Engineering Tiangong University Tianjin300387 China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China Tianjin and Ministry of Education Key Laboratory for Advanced Textile Composite Materials Tiangong University Tianjin300387 China Shaoxing keqiao Institute of Tiangong University Shaoxing3 12030 China Department of Bioinformatics and Medical Engineering Asia University Taichung413305 Taiwan Department of Medical Research China Medical University Hospital China Medical University Taichung City404333 Taiwan

Harvesting energy from naturally abundant water resources is expected to alleviate the need for the current energy shortage. However, existing studies rarely consider the effect of capacitors on the output of hydropower generation. Here, inspired by capacitors, we prepared a flexible and efficient hydrovoltaic generator by loading polypyrrole (PPy) and Ti3C2Tx MXene onto cotton fabrics by a simple green one-step synthesis method with self-assembly. Specifically, the ionic imbalance at the interface can be exacerbated by the use of expanded capacitance, while synergistically the two materials PPy/MXene will adsorb different ions, which promotes efficient adsorption of ions and ensures energy conversion. This generator can produce an open-circuit voltage (VOC) of 0.35 V and a short-circuit current (ISC) of ~260 μA in just 5 mL of a 3.5 wt% NaCl solution, and the optimized device can achieve an output power of 35.76 μW. Furthermore, this capacitance-enhanced fabric-based hydrovolt generator can directly power electronic devices and demonstrates its potential future applications in practical applications such as respiratory monitoring and touch sensing. © 2025

关键词： Fabrics

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