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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

Flexible Strain Sensors with Ultra-High Sensitivity and Wide Range Enabled by Crack-Modulated Electrical Pathways

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NANO-MICRO LETTERS 2025年第1期17卷 1-19页

作者： Bai, Yunzhao Zhou, Yunlei Wu, Xuanyu Yin, Mengfei Yin, Liting Qu, Shiyuan zhang, Fan Li, Kan Huang, Yongan Huazhong Univ Sci & Technol State Key Lab Intelligent Mfg Equipment & Technol Wuhan 430074 Peoples R China Huazhong Univ Sci & Technol Flexible Elect Res Ctr Wuhan 430074 Peoples R China Xidian Univ Hangzhou Inst Technol Hangzhou 311200 Peoples R China Xidian Univ Sch Mechanoelect Engn Xian 710071 Peoples R China Univ Southern Calif Dept Aerosp & Mech Engn Los Angeles CA 90089 USA

This study presents a breakthrough in flexible strain sensor technology with the development of an ultra-high sensitivity and wide-range sensor, addressing the critical challenge of reconciling sensitivity with measurement range. Inspired by the structure of bamboo slips, we introduce a novel approach that utilises liquid metal to modulate the electrical pathways within a cracked platinum fabric electrode. The resulting sensor demonstrates a gauge factor greater than 108 and a strain measurement capability exceeding 100%. The integration of patterned liquid metal enables customisable tuning of the sensor's response, while the porous fabric structure ensures superior comfort and air permeability for the wearer. Our design not only optimises the sensor's performance but also enhances the electrical stability that is essential for practical applications. Through systematic investigation, we reveal the intrinsic mechanisms governing the sensor's response, offering valuable insights for the design of wearable strain sensors. The sensor's exceptional performance across a spectrum of applications, from micro-strain to large-strain detection, highlights its potential for a wide range of real-world uses, demonstrating a significant advancement in the field of flexible electronics.

关键词： Flexible strain sensor Fabric Crack Response regulation Epidermal device

Bioinspired Ultrasensitive Flexible Strain Sensors for Real-Time Wireless Detection of Liquid Leakage

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NANO-MICRO LETTERS 2025年第1期17卷 1-18页

作者： Zhou, Weilong Du, Yu Chen, Yingying zhang, Congyuan Ning, Xiaowei Xie, Heng Wu, Ting Hu, Jinlian Qu, Jinping Huazhong Univ Sci & Technol Sch Chem & Chem Engn Key Lab Mat Chem Energy Convers & Storage Minist EducHubei Key Lab Mat Chem & Serv Failure Wuhan 430074 Peoples R China Huazhong Univ Sci & Technol Hubei Engn Res Ctr Biomat & Med Protect Mat Sch Chem & Chem Engn Wuhan 430074 Peoples R China Wuhan Inst Technol Sch Mat Sci & Engn Wuhan 430205 Peoples R China City Univ Hong Kong Dept Biomed Engn Hong Kong 999077 Peoples R China

Micro-extrusion compression molding and surface modification were proposed for the mass fabrication of a superhydrophobic thermoplastic polyurethane sensor (TCGS).Inspired by scorpions, TCGS features Archimedean spiral crack arrays and micropores, achieving 218.13 sensitivity at 2% strain, a 4300% increase, and over 5000 usage cycles of *** robust superhydrophobicity of TCGS improves sensitivity and stability for detecting small-scale liquid leakage, allowing precise monitoring across various sizes and compositions while providing early warnings in various scenarios. Liquid leakage of pipeline networks not only results in considerable resource wastage but also leads to environmental pollution and ecological imbalance. In response to this global issue, a bioinspired superhydrophobic thermoplastic polyurethane/carbon nanotubes/graphene nanosheets flexible strain sensor (TCGS) has been developed using a combination of micro-extrusion compression molding and surface modification for real-time wireless detection of liquid leakage. The TCGS utilizes the synergistic effects of Archimedean spiral crack arrays and micropores, which are inspired by the remarkable sensory capabilities of scorpions. This design achieves a sensitivity of 218.13 at a strain of 2%, which is an increase of 4300%. Additionally, it demonstrates exceptional durability by withstanding over 5000 usage cycles. The robust superhydrophobicity of the TCGS significantly enhances sensitivity and stability in detecting small-scale liquid leakage, enabling precise monitoring of liquid leakage across a wide range of sizes, velocities, and compositions while issuing prompt alerts. This provides critical early warnings for both industrial pipelines and potential liquid leakage scenarios in everyday life. The development and utilization of bioinspired ultrasensitive flexible strain sensors offer an innovative and effective solution for the early wireless detection of liquid leakage.

关键词： Thermoplastic polyurethane Bioinspired Cracks Liquid leakage Flexible strain sensor

Deciphering Water Oxidation Catalysts: The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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NANO-MICRO LETTERS 2025年第1期17卷 1-15页

作者： An, Li Li, Jianyi Sun, Yuanmiao Zhu, Jiamin Seow, Justin Zhu Yeow zhang, Hong zhang, Nan Xi, Pinxian Xu, Zhichuan J. Yan, Chun-Hua Lanzhou Univ Frontiers Sci Ctr Rare Isotopes Key Lab Nonferrous Met Chem & Resources Utilizat G State Key Lab Appl Organ ChemColl Chem & Chem Eng Lanzhou 730000 Peoples R China Nanyang Technol Univ Sch Mat Sci & Engn Singapore 639798 Singapore Chinese Acad Sci Fac Mat Sci & Energy Engn Shenzhen Inst Adv Technol Inst Technol Carbon Neutral Shenzhen 518055 Peoples R China Yunnan Univ Natl Ctr Int Res Photoelect & Energy Mat Electron Microscopy Ctr Sch Mat & EnergyKey Lab Electromagnet Mat & Devic Kunming 650091 Peoples R China Baotou Res Inst Rare Earths State Key Lab Baiyunobo Rare Earth Resource Res & Baotou 014030 Peoples R China Peking Univ Beijing Natl Lab Mol Sci State Key Lab Rare Earth Mat Chem & Applicat PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Chem Beijing 100871 Peoples R China

Demonstrate that the key factor to determine the activity of reconstructed surfaces is the surface chemistry, instead of reconstruction degree using the popular perovskite LaNi1-xFexO3 oxides as model *** content can influence both the surface reconstruction degree, the activation degree, and the activity of reconstructed *** oxygen evolution reaction activity of reconstructed catalysts is primarily governed by the chemistry of the reconstructed surface species. Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction. The surface reconstruction has been widely observed in perovskite catalysts, and the reconstruction degree has been often correlated with the activity enhancement. Here, a systematic study on the roles of Fe substitution in activation of perovskite LaNiO3 is reported. The substituting Fe content influences both current change tendency and surface reconstruction degree. LaNi0.9Fe0.1O3 is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi1-xFexO3 (x = 0.00, 0.10, 0.25, 0.50, 0.75, 1.00) series. The reconstructed LaNi0.9Fe0.1O3 shows a higher intrinsic activity than most reported NiFe-based catalysts. Besides, density functional theory calculations reveal that Fe substitution can lower the O 2p level, which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability. Furthermore, it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree. The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction. This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules

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Science China Chemistry 2025年第01期 264-272页

作者： Xueqing Ma Yingying Cheng Yuqiang Liu Xinming Zheng Guangliu Ran Hongxiang Li Xinyue Cui Andong zhang Wenkai zhang Pei Cheng Wenchao Huang Zhishan Bo Beijing Key Laboratory of Energy Conversion and Storage Materials College of Chemistry Beijing Normal University College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textiles Qingdao University Key State Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of Technology Department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum Studies Beijing Normal University State Key Laboratory of Polymer Materials Engineering College of Polymer Science and Engineering Sichuan University

Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells(OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene(EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene(DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-e C9-4F results in pre-aggregation and longer crystallization duration of BTP-e C9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in bladecoated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.

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An Efficient Boron Source Activation Strategy for the Low‑Temperature Synthesis of Boron Nitride Nanotubes

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Nano-Micro Letters 2025年第1期17卷 548-558页

作者： Ying Wang Kai zhang Liping Ding Liyun Wu Songfeng E Qian He Nanyang Wang Hui Zuo Zhengyang Zhou Feng Ding Yue Hu Jin zhang Yagang Yao National Laboratory of Solid State Microstructures College of Engineering and Applied SciencesJiangsu Key Laboratory of Artificial Functional Materialsand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093People’s Republic of China School of Electronic Information and Artificial Intelligence Shaanxi University of Science&TechnologyXian 710000People’s Republic of China College of Bioresources Chemical and Materials Engineering Shaanxi University of Science&TechnologyXian 710000People’s Republic of China Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325000People’s Republic of China Shenzhen Institutes of Advanced Technology Chinese Academy of SciencesShenzhen 518000People’s Republic of China College of Chemical and Molecular Engineering Peking UniversityBeijing 100871People’s Republic of China

Lowering the synthesis temperature of boron nitride nanotubes(BNNTs)is crucial for their *** primary reason for adopting a high temperature is to enable the effective activation of highmelting-point solid *** this study,we developed a novel approach for efficiently activating boron by introducing alkali metal compounds into the conventional MgO–B *** approach can be adopted to form various low-melting-point AM–Mg–B–O growth *** growth systems have improved catalytic capability and reactivity even under low-temperature conditions,facilitating the synthesis of BNNTs at temperatures as low as 850℃.In addition,molecular dynamics simulations based on density functional theory theoretically demonstrate that the systems maintain a liquid state at low temperatures and interact with N atoms to form BN *** findings offer novel insights into the design of boron activation and are expected to facilitate research on the low-temperature synthesis of BNNTs.

关键词： Boron nitride nanotubes Low-temperature Boron activation Density functional theory

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Co/Co_(7)Fe_(3)heterostructures with controllable alloying degree on carbon spheres as bifunctional electrocatalyst forrechargeable zinc-air batteries

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 476-487页

作者： Junkang Chen Yongyue Zhuang Yanxin Qiao Yu zhang Aihua Yuan Hu Zhou School of Materials Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying *** optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline *** intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co *** the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based *** particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending *** work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.

关键词： bifunctional electrocatalysts oxygen reduction reaction oxygen evolution reaction zinc-air battery metal/alloy carbon sphere

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Smart multi-functional aggregates reoxygenate tumor microenvironment through a two-pronged strategy to revitalize cancer immunotherapy

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Aggregate

Aggregate 2024年第4期5卷 256-268页

作者： Yan zhang luoqi Liang Hexiang Li Yuqing Cao Du Meng Xinru Li Meichen Wang Jingyuan Wang Yao Yao Shaoqiang zhang Chao Chen Peng Hou Qi Yang Key Laboratory for Tumor Precision Medicine of Shaanxi Province The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Department of Endocrinology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Department of Radiation Oncology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Department of Nuclear Medicine The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Medical Oncology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Department of Clinical Laboratory The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China Department of Otorhinolaryngology-Head and Neck Surgery The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anP.R.China

PD-1/PD-L1 inhibitors have emerged as standard treatments for advanced solid tumors;however,challenges such as a low overall response rate and systemic side effects impede their *** drives the remodeling of the tumor microenvironment,which is a leading reason for the failure of *** some reported strategies to alleviate hypoxia,their individual limitations constrain further ***,a novel two-pronged strategy is pre-sented to efﬁciently address hypoxia by simultaneously adopting atovaquone(ATO,inhibiting oxygen consumption)and oxyhemoglobin(HbO2,directly supplement-ing oxygen)within a multifunctional aggregate termed NPs-aPD-1/HbO2/*** addition to eliminating hypoxia with these two components,this smart aggre-gate also includes albumin and an ROS-responsive cross-linker as a controlled release scaffold,along with PD-1 antibody(aPD-1)for ***,NPs-aPD-1/HbO2/ATO demonstrates exceptional tumor targeting in vivo,exhibit-ing≈4.2 fold higher accumulation in tumors than in the ***,this aggregate not only effectively mitigates hypoxia and signiﬁcantly assists aPD-1 immunotherapy but also simultaneously resolves the targeting and systemic toxicity issues associated with individual administration of each *** study pro-poses substantial implications for drug-targeted delivery,addressing tumor hypoxia and advancing immunotherapy,providing valuable insights for advancing cancer treatment strategies.

关键词： hypoxia immunotherapy ROS-responsive smart aggregate synergistic therapy tumor targeting

Viscosity and structure relationship with equimolar substitution of CaO with MgO in the CaO–MgO–Al_(2)O_(3)–SiO_(2)slag melts

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 70-79页

作者： Yong Hou Shuo zhang Jie Dang Jia Guo Hanghang Zhou Xuewei Lü College of Materials Science and Engineering Chongqing UniversityChongqing 400044China Chongqing Key Laboratory of Vanadium-Titanium Metallurgy and New Materials Chongqing UniversityChongqing 400044China

Currently,the Al_(2)O_(3)content in the high-alumina slag systems within blast furnaces is generally limited to 16wt%–18.5wt%,making it challenging to overcome this *** most studies that concentrated on managing the MgO/Al_(2)O_(3)ratio or basicity,this paper explored the effect of equimolar substitution of MgO for CaO on the viscosity and structure of a high-alumina CaO-MgO-Al_(2)O_(3)-SiO_(2)slag system,providing theoretical guidance and data to facilitate the application of high-alumina *** results revealed that the viscosity first decreased and then increased with higher MgO substitution,reaching a minimum at 15mol%MgO *** transform infrared spectroscopy(FTIR)results found that the depths of the troughs representing[SiO_(4)]tetrahedra,[AlO_(4)]tetrahedra,and Si-O-Al bending became progressively deeper with increased MgO *** of the Raman spectra showed that the average number of bridging oxygens per Si atom and the X_(Q^(3))/X_(Q^(2))(X_(Q^(i))is the molar fraction of Q^(i) unit,and i is the number of bridging oxygens in a[SiO_(4)]tetrahedral unit)ratio increased from 2.30 and 1.02 to 2.52 and 2.14,respectively,indicating a progressive polymerization of the silicate structure.X-ray photoelectron spectroscopy(XPS)results highlighted that non-bridging oxygen content decreased from 77.97mol% to 63.41mol% with increasing MgO concentration,whereas bridging oxygen and free oxygen contents *** analysis demonstrated a gradual increase in the polymerization degree of the tetrahedral structure with the increase in MgO ***,bond strength is another important factor affecting the slag *** occurrence of a viscosity minimum can be attributed to the complex evolution of bond strengths of non-bridging oxygens generated during depolymerization of the[SiO_(4)]and[AlO_(4)]tetrahedral structures by CaO and MgO.

关键词： aluminosilicate viscosity structure spectroscopy

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