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materials Today Catalysis 2024年 7卷

作者： Meng, Youcai Ding, Junyang Liu, Yifan Hu, Guangzhi Feng, Yanhong Wu, Yinghong Liu, Xijun MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials School of Resources Environment and Materials Guangxi University Nanning530004 China Institute of Advanced Science Facilities Guangdong Shenzhen518107 China Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental Science Yunnan University Kunming650504 China National Engineering Research Center of Green Recycling for Strategic Metal Resources Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Group Department of Health Sciences and Technology ETH Zürich Zürich8008 Switzerland

Electrocatalytic CO2 reduction (ECR) is a crucial energy conversion technology that transforms CO2 into value-added chemicals, reducing reliance on fossil fuels and advancing energy transitions. Designing high-performance catalysts is pivotal for widespread adoption of CO2 reduction reactions, aiming for high activity, selectivity, and stability. Amorphous oxides represent a burgeoning frontier in this field, attracting attention due to their abundant active sites that refine the catalyst structure-performance relationship. This paper aims to provide an overview of recent advances in using amorphous oxides for ECR. We begin by introducing the basic theory of electrocatalytic CO2 reduction, followed by discussing current synthesis approaches for amorphous oxides in CO2 reduction, focusing on optimization strategies for these catalysts. Finally, we address challenges and future perspectives of amorphous oxides in ECR, aiming to foster the development of more efficient catalyst designs. © 2024 The Authors

关键词： Catalyst selectivity

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Hypervalent Potassium Xanthate Modified Sno2 for Highly Efficient Perovskite Solar Modules

SSRN

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SSRN 2022年

作者： Lu, Jianfeng Lv, Pin Yang, Yufei Li, Neng Zhang, Yuxi Hu, Min Huang, Bo Zhu, Yanqing Li, Bin Pan, Junye Wang, Shifeng Huang, Fuzhi Cheng, Yi-Bing State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology Wuhan430070 China School of Electronic and Electrical Engineering Hubei Province Engineering Research Center for Intelligent Micro-Nano Medical Equipment and Key Technologies Wuhan Textile University Wuhan430200 China Foshan Xianhu Laboratory The Advanced Energy Science and Technology Guangdong Laboratory Foshan528216 China Innovation Laboratory of Materials for Energy and Environment Technologies Institute of Oxygen Supply Tibet University Lhasa850000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

Tin oxide (SnO2) has been demonstrated as a promising electron transport material for high efficiency perovskite solar cells (PSCs) that made entirely via solution processing at low temperature (2|perovskite lead to a large voltage loss and performance variation. Herein, we present a facile and effective method to simultaneously reduce the interfacial defects and enhance the charge transfer via modification of SnO2 by hypervalent potassium xanthate. The presence of Lewis acidic centers of the sulfur ligands, gives rise to a strong hypervalent interactions with both Pb2+ on the perovskite and Sn4+ on the SnO2 surface, which accelerates the interfacial charge transfer and suppresses the recombination reaction. As a result, solar cells with a power conversion efficiency of 23.4% with negligible hysteresis are fabricated in light of significantly increased voltage in comparison with the relevant controls. Moreover, a stabilized efficiency of 18.8% for large-area (active area: 48.0 cm2) perovskite solar modules is achieved. The modules retain 90% of their initial performance after aging at ambient for 600 hours, which is substantially improved in comparison with the modules based on pristine SnO2 © 2022, The Authors. All rights reserved.

关键词： Perovskite solar cells

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The Multidimensional Optimization Effects of L-Serine in the Mineralization of Carbide Slag and the Controllable Synthesis of Novel and Unique Caco3 Morphologies

SSRN

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SSRN 2025年

作者： Gao, Peng Wu, Xiao He, Quan Li, Qingping Wang, Pengfei Zhang, Lunxiang Zhao, Jiafei Song, Yongchen Yang, Lei Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education Dalian University of Technology Dalian116024 China State Key Laboratory of Natural Gas Hydrates Beijing100028 China Ningbo Institute of Dalian University of Technology Ningbo315016 China Shenzhen Key Laboratory of Natural Gas Hydrate Department of Physics Institute of 13 Major Scientific Facilities for New Materials Academy for Advanced Interdisciplinary 14 Studies Southern University of Science and Technology Shenzhen518055 China

Technologies for resource use and carbon neutrality have been identified as crucial avenues for reducing the rising atmospheric CO2 concentration as global climate change intensifies. Among these, CO2 mineralization and sequestration technology is becoming more and more recognized as a successful carbon reduction technique. With an emphasis on the mechanisms affecting calcium ion leaching, mineralization processes, and product morphology regulation, this study examined the multidimensional optimization impacts of L-serine in the mineralization of carbide slag (CS). With a leaching rate of 90.6% at a concentration of 5 mol/L, it was shown that the addition of L-serine greatly increased the effectiveness of calcium ion leaching. CO2 fixation of 554 kg per ton of carbide slag was achieved during the mineralization phase by reducing the reaction induction time and significantly increasing the mineralization rate. Additionally, L-serine controlled the shape of CaCO3 crystals, promoting the transition from calcite to vaterite and, in excess, forming distinctive spherical calcite structures with extremely high hardness and enhanced thermal stability. Although a transition effect in L-serine's regenerative performance was found, cyclic studies showed the protein's capacity for regeneration. These findings offer new information and technical assistance for the fabrication of high-performance CaCO3 materials and the resource exploitation of carbide slag. © 2025, The Authors. All rights reserved.

关键词： Carbide minerals

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Role of transport polarization in electrocatalysis:A case study of the Ni-cluster/Graphene interface

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Journal of materials Science & technology 2021年第33期92卷 120-128页

作者： Fang Bian Xin Ge Wu Shan Shan Li Gao Wu Qin Xiang Ying Meng Yin Wang Hong Wei Yang School of Materials Science and Engineering Northeastern UniversityShenyang 110819China College of Sciences Northeastern UniversityShenyang 110819China Research Center for Metallic Wires Northeastern UniversityShenyang 110819China The State Key Laboratory of Rolling and Automation Northeastern UniversityShenyang 110819China International Centre of Quantum and Molecular Structures and Department of Physics Shanghai UniversityShanghai 200444China State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum Metals Kunming Precious Metals New Materials Technology Co.Ltd.Kunming 650106China

As cathodes,iron-series(Fe,Co,Ni)clusters supported by carbon materials exhibit outstanding electrocatalytic reduction activities in many electrocatalytic *** date,this general characteristic of ironseries clusters that should be related to the inherent attributes of these electrodes has not been fully understood from the perspectives of thermodynamics and electronic structure *** transport is a necessary process in electrocatalysis,and therefore,the study of the change of the electronic state in electron transport is beneficial for understanding this general characteristic of iron-series cluster *** this work,the electron transport properties,including the conductivity and transport spin-polarization at the Ni-cluster/graphene interface are carefully investigated as an example of carbon-supported iron-series *** first-principles calculations within the framework of the nonequilibrium Green’s function density functional theory(NEGF-DFT),we reveal that the electronic transport states of the coupled Ni-cluster/graphene are strongly changed compared to those of their isolated Ni-cluster and graphene *** is found that graphene dominates the overall conductivity of the interface,while the morphology of Ni-clusters controls the spin polarization *** spin polarization can lead to the self-excitation effect of the electrons that raises the energy of the electronic system,improves the thermodynamics of the reduction reaction and promotes catalytic *** work hints that iron-series elements(Fe,Co,Ni)based electrodes may generally show transport polarization that is likely to give rise to a high electrocatalytic reduction activity and such transport polarizability can be used as a new factor in the further exploration and design for electrocatalytic materials.

关键词： First-principles calculations electrocatalysis non-equilibrium electron injection transport polarization Ni-cluster/graphene

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A chitosan derivative-crosslinked hydrogel with controllable release of polydeoxyribonucleotides for wound treatment

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Carbohydrate Polymers 2023年 300卷 120298页

作者： Sun, Yanzhen Jing, Xiaodong Liu, Yang Yu, Bing Hu, Hao Cong, Hailin Shen, Youqing Institute of Biomedical Materials and Engineering College of Chemistry and Chemical Engineering College of Materials Science and Engineering Qingdao University Qingdao266071 China Laboratory for New Fiber Materials and Modern Textile Growing Base for State Key Laboratory Qingdao University Qingdao266071 China School of Materials Science and Engineering Shandong University of Technology Zibo266071 China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Center for Bionanoengineering Department of Chemical and Biological Engineering Zhejiang University Hangzhou310027 China

Nucleic acid-based agents have advantages in therapeutic efficacy and biological safety. However, due to its facile degradability, it lacks an effective route of administration in wound treatment. Designing smart hydrogels for the spatiotemporally controllable delivery of nucleic acids is of great significance for clinical applications. Here, a near-infrared (NIR)-responsive nanocomposite hydrogel was prepared using methyl methacrylate (GMA)-modified chitosan as the macromolecular cross-linker, N-isopropylacrylamide (NIPAAm) as the backbone, and molybdenum disulfide nanosheets (MoS2 NSs) as the nanocomponents. The polydeoxyribonucleotide (PDRN), a nucleic acid-based agent that promotes tissue regeneration, was loaded and delivered. The photothermal conversion capability of MoS2 NSs enables customized care of PDRNs and antibacterial enhancement. In a full-thickness skin defect model, high-quality wound healing effects were demonstrated under the action of nanocomposite hydrogels. The proposed nanocomposite hydrogel provides a new reference for local delivery of nucleic acid-based agents. © 2022 Elsevier Ltd

关键词： Controlled drug delivery

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Finite-temperature properties of antiferroelectric perovskite PbZrO3 from deep learning interatomic potential

arXiv

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arXiv 2024年

作者： Zhang, Huazhang Thong, Hao-Cheng Bastogne, Louis Gui, Churen He, Xu Ghosez, Philippe Theoretical Materials Physics Q-MAT University of Liège Sart-Tilman B-4000 Belgium Department of Physics School of Science Wuhan University of Technology Wuhan430070 China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China Key Laboratory of Quantum Materials and Devices of Ministry of Education School of Physics Southeast University Nanjing211189 China

The prototypical antiferroelectric perovskite PbZrO3 (PZO) has garnered considerable attentions in recent years due to its significance in technological applications and fundamental research. Many unresolved issues in PZO are associated with large length- and time-scales, as well as finite temperatures, presenting significant challenges for first-principles density functional theory studies. Here, we introduce a deep learning interatomic potential of PZO, enabling investigation of finite-temperature properties through large-scale atomistic simulations. Trained using an elaborately designed dataset, the model successfully reproduces a large number of phases, in particular, the recently discovered 80-atom antiferroelectric Pnam phase and ferrielectric Ima2 phase, providing precise predictions for their structural and dynamical properties. Using this model, we investigated phase transitions of multiple phases, including Pbam/Pnam, Ima2 and R3c, which show high similarity to the experimental observation. Our simulation results also highlight the crucial role of free-energy in determining the low-temperature phase of PZO, reconciling the apparent contradiction: Pbam is the most commonly observed phase in experiments, while theoretical calculations predict other phases exhibiting even lower energy. Furthermore, in the temperature range where the Pbam phase is thermodynamically stable, typical double polarization hysteresis loops for antiferroelectrics were obtained, along with a detailed elucidation of the structural evolution during the electric-field induced transitions between the non-polar Pbam and polar R3c phases. © 2024, CC BY.

关键词： Free energy

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High-Pressure And High-Temperature Synthesis of Black Phosphorus-Graphite Anode Material for Lithium-Ion Batteries

SSRN

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SSRN 2023年

作者： Cheng, Zhikang Tu, Bingtian Wu, Ye Huang, Haijun School of Science Wuhan University of Technology Hubei Wuhan430070 China Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration Zone Hubei Xiangyang441000 China State Key Lab of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China

Phosphorus-based materials with a high theoretical specific capacity and a fast charge-discharge rate are considered as promising anode materials for high energy density lithium-ion batteries (LIBs). Red phosphorus (RP) and black phosphorus (BP) are two main allotropes to be used as anode materials. However, huge volume expansion during charge-discharge processes hinders the application of RP and BP in LIBs. Composites of phosphorus and carbon-based materials have been extensively fabricated to withstand volume expansion of phosphorus and improve cycle performance. Here, composites of BP and graphite (BP-G) with three P-G mass ratios (8 : 2, 7 : 3, and 6 : 4) have been synthesized by a facile and scalable high-pressure and high-temperature (HPHT) method using RP and graphite composites (RP-G) prepared by ball milling as precursors. Their microstructure and bonding configurations have been analyzed by various characterization techniques. Among three RP-G composites, 7RP-3G exhibits the most excellent cycling stability, a high reversible capacity of 1331 mAh/g after 200 cycles at a current density of 0.78 A/g. However, RP-G composites show poor stability at high current densities. Among three BP-G composites, 6BP-4G shows the best cycle stability at high current densities, a reversible capacity of 634.6 mAh/g after 500 cycles at a current density of 2.6 A/g. Although, the reversible specific capacities of BP-G composites after long cycles are lower than those of RP-G, BP-G composites show more stable cycle performance than RP-G, especially at high current densities. The present work illustrates a direct and facile method to synthesize BP-G composites, and sheds light to explore new synthetic route of BP-based composites. © 2023, The Authors. All rights reserved.

关键词： Lithium-ion batteries

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Tuning Ferroelectrics to Antiferroelectrics in Multiferroic LaxSr1-xFe12O19 Ceramics

arXiv

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arXiv 2021年

作者： Duan, Cong-Cong Tan, Guo-Long State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

The combination of antiferroelectricity (AFE) and ferromagnetism (FM) in one structure would allow the development of new type of multiferroic candidates, which be applicable not only in magnetoelectric memories but also in novel energy storage devices. Here we propose a novel type of multiferroic candidate LaxSr1-xFe12O19, whose room temperature state could betuned from ferroelectrics (FE) to antiferroelectrics by changing x from 0 to 0.5. The emphasis of this paper will be focused on the La0.5Sr0.5Fe12O19 system, in which full AFE and FM coexist. The pure antiferroelectric behavior in La0.5Sr0.5Fe12O19 ceramics is demonstrated by double polarization-electric field (P-E) hysteresis loops, which are fully separated by a linear antiferroelectric AFE component with zero net polarization. The material of La0.2Sr0.7Fe12O19 with the intermediate composition exhibits a hybrid ferroelectric/antiferroelectric state. The recoverable energy density of the antiferroelectric La0.5Sr0.5Fe12O19 phase reaches Ure∼14.3 J/cm3. This material demonstrates strong magnetoelectric coupling and giant magnetoresistance (GMR) effect. A 1.1T magnetic field generates electronic polarization up to 0.95μC/cm2, reduce the resistance by 117%, enhances dielectric constants by 540% and right shifts the maximum dielectric loss peak by 208 kHz. The combined functional responses provide an opportunity to develop novel multifunctional electric and energy storage devices. © 2021, CC BY.

关键词： Energy storage

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Anomalous Nernst Effect in an Antiperovskite Antiferromagnet

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Physical Review Applied 2022年第2期18卷 024007-024007页

作者： Yunfeng You Hei Lam Caihua Wan Chunlei Wan Wenxuan Zhu Lei Han Hua Bai Yongjian Zhou Leilei Qiao Tongjin Chen Feng Pan Junwei Liu Cheng Song Key Laboratory of Advanced Materials School of Materials Science and Engineering Tsinghua University Beijing 100084 China Department of Physics Hong Kong University of Science and Technology Hong Kong 00852 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China

The anomalous Nernst effect (ANE), the generation of a transverse electric voltage by a longitudinal temperature gradient, has attracted increasing interest from researchers recently, due to its potential in thermoelectric power conversion and close relevance to the Berry curvature of the band structure. Avoiding the stray field of ferromagnets, the ANE in antiferromagnets (AFMs) has the advantage of realizing highly efficient and densely integrated thermopiles. Here, we report the observation of the ANE in an antiperovskite noncollinear AFM, Mn3SnN, experimentally, which is triggered by the enhanced Berry curvature from Weyl points located close to the Fermi level. Considering that antiperovskite Mn3SnN has a rich magnetic phase transition, we modulate the noncollinear AFM configurations by the biaxial strain, which enables us to control its ANE. Our findings provide a potential class of materials to explore the Weyl physics of noncollinear AFMs as well as realizing antiferromagnetic spin caloritronics that exhibits promising prospects for energy conversion and information processing.

关键词： Electronic structure Magnetic phase transitions Magnetotransport Nernst effect Spin caloritronics Thermoelectric generators Antiferromagnets Noncollinear magnets

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Linker Mediated Electronic-state Manipulation of Conjugated Organic Polymers Enabling Highly Efficient Oxygen Reduction

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Angewandte Chemie 2024年第26期136卷

作者： Rui Ma Chenglong Tang Yonglin Wang Xiaoxue Xu Prof. Mingjie Wu Prof. Xun Cui Prof. Yingkui Yang State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 China School of Chemistry and Materials Science South-Central Minzu University Wuhan 430074 China

Conjugated polymers with tailorable composition and microarchitecture are propitious for modulating catalytic properties and deciphering inherent structure-performance relationships. Herein, we report a facile linker engineering strategy to manipulate the electronic states of metallophthalocyanine conjugated polymers and uncover the vital role of organic linkers in facilitating electrocatalytic oxygen reduction reaction (ORR). Specifically, a set of cobalt phthalocyanine conjugated polymers (CoPc-CPs) wrapped onto carbon nanotubes (denoted CNTs@CoPc-CPs) are judiciously crafted via in situ assembling square-planar cobalt tetraaminophthalocyanine (CoPc(NH 2 ) 4 ) with different linear aromatic dialdehyde-based organic linkers in the presence of CNTs. Intriguingly, upon varying the electronic characteristic of organic linkers from terephthalaldehyde (TA) to 2,5-thiophenedicarboxaldehyde (TDA) and then to thieno/thiophene-2,5-dicarboxaldehyde (bTDA), their corresponding CNTs@CoPc-CPs exhibit gradually improved electrocatalytic ORR performance. More importantly, theoretical calculations reveal that the charge transfer from CoPc units to electron-withdrawing linkers (i.e., TDA and bTDA) drives the delocalization of Co d-orbital electrons, thereby downshifting the Co d-band energy level. Accordingly, the active Co centers with more positive valence state exhibit optimized binding energy toward ORR-relevant intermediates and thus a balanced adsorption/desorption pathway that endows significant enhancement in electrocatalytic ORR. This work demonstrates a molecular-level engineering route for rationally designing efficient polymer catalysts and gaining insightful understanding of electrocatalytic mechanisms.

关键词： linker engineering electronic-state manipulation cobalt phthalocyanine conjugated polymer oxygen reduction reaction

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