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Divalent anion intercalation and etching-hydrolysis strategies to construct ultra-stable electrodes for seawater splitting

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Science China Chemistry 2024年第2期67卷 687-695页

作者： jiajia Lu yang Liu Han-Pu Liang Key Laboratory of Biofuels Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao266101China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nano-Structured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou450006China School of Materials Science and Engineering Henan Normal UniversityXinxiang453007China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China Shandong Energy Institute Qingdao266101China

Developing stable electrodes for seawater splitting remains a great challenge due to the detachment of catalysts at a large operating current and severe anode corrosion caused by chlorine.Herein,divalent anion intercalation and etching-hydrolysis strategies are deployed to synthesize the ultra-stable anode,dendritic Fe(OH)_(3) grown on Ni(SO_4)_(0.3)(OH)_(1.4)–Ni(OH)_(2).Experimental results reveal that the anode exhibits good activity and excellent stability in alkaline simulated seawater.After 500 h,the current density operated at 1.72 V remains 99.5%,about 210 m A cm^(-2).The outstanding stability originates from the etchinghydrolysis strategy,which strengthens the interaction between the catalyst and the carrier and retards thus the detachment of catalysts at a large current density.Besides,theoretical simulations confirm that the intercalated divalent anions,such as SO_4^(2-) and CO_(3)^(2-),can weaken the adsorption strength of chlorine on the surface of catalysts and hinder the coupling and hybridization between chlorine and nickel,which slows down the anode corrosion and improves catalytic stability.Furthermore,the twoelectrode system shows the remarkable 95.1% energy efficiency at 2,000 A m-2and outstanding stability in 6 mol L^(-1) KOH +seawater at 80 ℃.

关键词： seawater splitting stability divalent anion intercalation etching-hydrolysis

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Patterning single-layer materials by electrical breakdown using atomic force microscopy

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Nanotechnology and Precision Engineering 2024年第1期7卷 71-77页

作者： Yajie yang jiajia Lu Yanbo Xie Libing Duan School of Physical Science and Technology Northwestern Polytechnical UniversityXi’an 710072China School of Aeronautics and Institute of Extreme Mechanics Northwestern Polytechnical UniversityXi’an 710072China

The development of nanoelectronics and nanotechnologies has been boosted signiﬁcantly by the emergence of 2D materials because of their atomic thickness and peculiar properties,and developing a universal,precise patterning technology for single-layer 2D materials is critical for assembling nanodevices.Demonstrated here is a nanomachining technique using electrical breakdown by an AFM tip to fabricate nanopores,nanostrips,and other nanostructures on demand.This can be achieved by voltage scanning or applying a constant voltage while moving the tip.By measuring the electrical current,the formation process on single-layer materials was shown quantitatively.The present results provide evidence of successful pattern fabrication on single-layer MoS2,boron nitride,and graphene,although further conﬁrmation is still needed.The proposed method holds promise as a general nanomachining technology for the future.

关键词： 2D material Nanopattern AFM Electrical breakdown Lithography

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MIL-100(V) derived porous vanadium oxide/carbon microspheres with oxygen defects and intercalated water molecules as high-performance cathode for aqueous zinc ion battery

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Journal of Energy Chemistry 2024年第3期90卷 578-589,I0013页

作者： Yuexin Liu Jian Huang Xiaoyu Li jiajia Li Jinhu yang Kefeng Cai Shanghai Key Laboratory of Development and Application for Metal-Functional Materials Key Laboratory of Advanced Civil Engineering MaterialsMinistry of EducationSchool of Materials Science&EngineeringTongji UniversityShanghai 201804China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 201800China Research Center for Translational Medicine East HospitalTongji University School of MedicineShanghai 200092China

The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.

关键词： Metal-organic frameworks Vanadium oxide Carbon Zn-ion batteries Electrochemical activation

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Macrophage senescence in health and diseases

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Acta Pharmaceutica Sinica B 2024年第4期14卷 1508-1524页

作者： Longling Wang Wenxiang Hong Hong Zhu Qiaojun He Bo yang jiajia Wang Qinjie Weng Center for Drug Safety Evaluation and Research Zhejiang Province Key Laboratory of Anti-Cancer Drug ResearchCollege of Pharmaceutical SciencesZhejiang UniversityHangzhou 310058China Nanhu Brain-Computer Interface Institute Hangzhou 311100China Taizhou Institute of Zhejiang University Taizhou 318000China The Second Affiliated Hospital Zhejiang University School of MedicineHangzhou 310009China

Macrophage senescence,manifested by the special form of durable cell cycle arrest and chronic low-grade inflammation like senescence-associated secretory phenotype,has long been consid-ered harmful.Persistent senescence of macrophages may lead to maladaptation,immune dysfunction,and finally the development of age-related diseases,infections,autoimmune diseases,and malignancies.However,it is a ubiquitous,multi-factorial,and dynamic complex phenomenon that also plays roles in remodeled processes,including wound repair and embryogenesis.In this review,we summarize some general molecular changes and several specific biomarkers during macrophage senescence,which may bring new sight to recognize senescent macrophages in different conditions.Also,we take an in-depth look at the functional changes in senescent macrophages,including metabolism,autophagy,polarization,phagocytosis,antigen presentation,and infiltration or recruitment.Furthermore,some degenerations and diseases associated with senescent macrophages as well as the mechanisms or relevant genetic regulations of senescent macrophages are integrated,not only emphasizing the possibility of regulating macrophage senescence to benefit age-associated diseases but also has an implication on the finding of potential tar-gets ordrugs clinically.

关键词： Macrophages Senescence Molecular changes Functional alterations Aging tissues Age-associated diseases Drug treatment Genetic regulation

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Bionic immunoactivator copresenting autophagy promoting and costimulatory molecules for synergistic cancer immunotherapy

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Nano Research 2024年第3期17卷 1710-1724页

作者： Yiwei Peng Yiliang yang Zhenzhen yang Datong Gao jiajia Li Qi Sun Yitian Du Meng Lin Xianrong Qi Beijing Key Laboratory of Molecular Pharmaceutics and New Drug Delivery System School of Pharmaceutical SciencesPeking UniversityBeijing 100191China

Immunotherapy has great promise in improving malignant tumor treatment.However,the efficacy of existing strategies is often limited by the immunosuppressive environment.Here,we demonstrate an in situ bionic immunoactivator,PLT-Bec1/DTA-1,with possessed natural advantages of platelets for tumor recruitment and activation,on which DTA-1(CD357 monoclonal antibody)and Bec1 were tethered as combined immune boosters.PLT-Bec1/DTA-1,as a self-triggered release repository,can deliver the pre-tethered Bec1 and DTA-1 deeply through the secretion of platelet microparticles(PMPs),thereby cooperate tacitly and exhibit superiority in immune activation of dendritic cells(DCs)and T cells via autophagy inducibility,coupled with glucocorticoid-induced tumor necrosis factor receptor(GITR)-triggered T_(Reg) suppression,remodeled the immunosuppressive network of tumor microenvironment.PLT-Bec1/DTA-1 promoted antigen presentation and T cell proliferation,and alleviated the low activity state of bone marrow-derived dendritic cells(BMDCs)in tumor suppressive environment.PLT-Bec1/DTA-1 inhibited tumor recurrence(5-and 13-fold lower of control group in tumor volume)and CD8^(+)T/T_(Reg) ratio(6.3-and 8.8-fold vs.control group)in mouse tumor model after intravenous or subcutaneous administration.Also,PLT-Bec1/DTA-1 prevented tumor colonization in lung through in situ immune activation,and was slightly superior to the combined of Bec1 and PD-L1.Our findings highlight the promise of delivering immunostimulatory payloads via bionic carriers,eliciting automatic in situ activation of effector immune cells in tumor microenvironment for tumor eradication.All these results provide promising prospects into the application of immunoactivator in improving cancer synergistic immunotherapy to overcome the bottlenecks in clinic.

关键词： in situ bionic immunoactivator autophagy glucocorticoid-induced tumor necrosis factor receptor(GITR)agonist platelets and platelet microparticles cancer immunotherapy

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Ribosome-inspired electrocatalysts inducing preferential nucleation and growth of three-dimensional lithium sulfide for high-performance lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第7期94卷 517-526页

作者： Zhen Wu Wenfeng He Jiahui yang Yunuo Gu Ruiqi yang Yiran Sun jiajia Yuan Xin Wang Junwu Zhu Yongsheng Fu Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094JiangsuChina School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina FEB Res Inst Far East BatteryWuxi 214200JiangsuChina

Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle effect.However,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its nucleation.In this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)electrocatalysts.Excitedly,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during discharge.Theoretical calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle effect.This study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.

关键词： Lithium-sulfur batteries Electrocatalysts Nanocrystals Ribosome-inspired Nucleation and growth

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Rapid and chemoselective imidation of sulfides in aqueous buffer enabled by a novel guanidine-derived N-O reagent

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Science China Chemistry 2024年第6期67卷 1929-1934页

作者： Hanzheng Li Long Xu jiajia Dong Key Laboratory of Organofluorine Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032China Institute of Translational Medicine National Facility for Translational Medicine(Shanghai)Shanghai Jiao Tong UniversityShanghai200240China School of Chemistry and Chemical Engineering Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai200240China Shanghai Artificial Intelligence Laboratory Shanghai200232China

Herein we report the facile synthesis of a series of novel N-O reagents and identify N′-di-Boc-N′′-[(mesitylsulfonyl)oxy]-guanidine as an efficient imidating reagent.This reagent is synthetically scalable and bench-stable,yet it shows unprecedented reactivity and chemoselectivity towards S(II)in buffer/hexafluoroisopropanol(HFIP)system,to generate a new class of Nguanyl sulfilimines.Further transformation of N-guanyl sulfilimines to N-guanyl sulfoximines provides us a chance to investigate these rarely reached compounds,which are shown to be versatile precursors to a variety of N-heterocyclic and NHsulfoximines.Our work provides an addition to the tool box of both sulfur imidation and guanidine synthesis,especially for the need of rapid and selective modifications of sulfur(II)center under biocompatible conditions.

关键词： sulfur imidation N-O reagent

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Metabolic plasticity of T cell fate decision

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中华医学杂志(英文版) 2024年第7期137卷 762-775页

作者： Pan Xiaoli Wang jiajia Zhang Lianjun Li Guideng Huang Bo Institute of Basic Medical Sciences Chinese Academy of Medical Sciences (CAMS) & Beijing 100005 National Key Laboratory of Immunity and Inflammation Suzhou Institute of Systems Medicine Chinese Academy of Medical Sciences & Peking Union Medical College Suzhou Jiangsu 215123 China Department of Immunology & National Key Laboratory of Medical Molecular Biology

The efficacy of adaptive immune responses in cancer treatment relies heavily on the state of the T cells. Upon antigen exposure, T cells undergo metabolic reprogramming, leading to the development of functional effectors or memory populations. However, within the tumor microenvironment (TME), metabolic stress impairs CD8+ T cell anti-tumor immunity, resulting in exhausted differentiation. Recent studies suggested that targeting T cell metabolism could offer promising therapeutic opportunities to enhance T cell immunotherapy. In this review, we provide a comprehensive summary of the intrinsic and extrinsic factors necessary for metabolic reprogramming during the development of effector and memory T cells in response to acute and chronic inflammatory conditions. Furthermore, we delved into the different metabolic switches that occur during T cell exhaustion, exploring how prolonged metabolic stress within the TME triggers alterations in cellular metabolism and the epigenetic landscape that contribute to T cell exhaustion, ultimately leading to a persistently exhausted state. Understanding the intricate relationship between T cell metabolism and cancer immunotherapy can lead to the development of novel approaches to improve the efficacy of T cell-based treatments against cancer.

关键词： T cell immunotherapy T cell differentiation T cell exhaustion Metabolic reprogramming Tumor microenvironment

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Characteristics and influencing factors of greenhouse gas emissions from reservoirs in the Yellow River Basin:A Meta-analysis

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Science China Earth Sciences 2024年第7期67卷 2210-2225页

作者： Shurui HUANG Peijia ZHANG Wenxiu ZHENG jiajia ZHANG yang LI Yuanjian WANG Enhui JIANG Shaoda LIU Xinghui XIA State Key Laboratoy of Water Environment Simulation School of EnvironmentBeijing Normal UniversityBeijing 00875China Yellow River Institute of Hydraulic Research Yellow River Conservancy CommissionZhengzhou 450003China

Reservoir construction and operation profoundly alter the hydrological,hydrodynamic,and carbon and nitrogen cycling processes of rivers.However,current research still lacks a systematic understanding of the characteristics of greenhouse gas(GHG)emissions from reservoirs in arid/semi-arid regions.This study integrates existing monitoring data to discuss the characteristics of GHG emissions from reservoirs in the Yellow River Basin and illustrate the controlling factors and underlying mechanism of these processes.The results indicate that while CO_(2) emission flux from reservoirs is lower than that from river channels,the emission fluxes of CH_(4) and N_(2)O are 1.9 times and 10 times those from rivers,respectively,indicating that the emission of GHG with stronger radiative effect is significantly enhanced in reservoirs.Compared to the reservoirs in humid climates(e.g.,the Three Gorges Reservoir),reservoirs in the Yellow River Basin exhibit relatively lower emissions of CO_(2) and CH_4 due to lower organic matter concentrations,but significantly higher N_(2)O emissions due to higher nitrogen loads.Monte Carlo simulations for 237 reservoirs in the Yellow River Basin showed that total emission of the three GHGs is 3.05 Tg CO_(2)-eq yr^(-1),accounting for 0.39% of the total emission from global reservoirs and lower than the area percentage of the basin(0.53%).This study has important implications on revealing the GHG emission characteristics and control mechanisms of reservoirs in arid/semi-arid regions.

关键词： Yellow River Basin Reservoir Greenhouse gas Emission flux Water quality

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Insights into Nano-and Micro-Structured Scaffolds for Advanced Electrochemical Energy Storage

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Nano-Micro Letters 2024年第7期16卷 187-230页

作者： jiajia Qiu Yu Duan Shaoyuan Li Huaping Zhao Wenhui Ma Weidong Shi Yong Lei Fachgebiet Angewandte Nanophysik Institut Für Physik and IMN MacroNanoTechnische Universit.t Ilmenau98693 IlmenauGermany Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Faculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093People’s Republic of China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013People’s Republic of China School of Science and Technology Pu’er UniversityPu’er 665000People’s Republic of China

Adopting a nano-and micro-structuring approach to fully unleashing the genuine potential of electrode active material benefits in-depth understandings and research progress toward higher energy density electrochemical energy stor-age devices at all technology readiness levels.Due to various challenging issues,especially limited stability,nano-and micro-structured(NMS)electrodes undergo fast electrochemical performance degradation.The emerging NMS scaffold design is a pivotal aspect of many electrodes as it endows them with both robustness and electrochemical performance enhancement,even though it only occupies comple-mentary and facilitating components for the main mechanism.However,extensive efforts are urgently needed toward optimizing the stereoscopic geometrical design of NMS scaffolds to minimize the volume ratio and maximize their functionality to fulfill the ever-increasing dependency and desire for energy power source supplies.This review will aim at highlighting these NMS scaffold design strategies,summariz-ing their corresponding strengths and challenges,and thereby outlining the potential solutions to resolve these challenges,design principles,and key perspectives for future research in this field.Therefore,this review will be one of the earliest reviews from this viewpoint.

关键词： Nano-and micro-structured Interconnected porous Scaffolds Electrode design Electrochemical energy storage

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