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Strategies to achieve effective nitrogen activation

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Carbon Energy 2024年第5期6卷 137-163页

作者： Bin Chang Huabin Zhang shuhui sun Gaixia Zhang KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalKingdom of Saudi Arabia Institut National de la Recherche Scientifique(INRS) CentreÉnergie Matériaux TélécommunicationsVarennesQuébecCanada Department of Electrical Engineering École de Technologie Supérieure(ÉTS)MontréalQuébecCanada

Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.

关键词： activation via mediators catalyst optimization electrochemical nitrogen fixation high-energy activation of nitrogen nitrogen

Advancements on metal oxide semiconductor photocatalysts in photo-electrochemical conversion of carbon dioxide into fuels and other useful products

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Frontiers in Energy 2024年第2期18卷 187-205页

作者： Jai PRAKASH Zhangsen CHEN Shakshi SAINI Gaixia ZHANG shuhui sun Department of Chemistry National Institute of Technology HamirpurHamirpur 177005India Institut National de la Recherche Scientifique(INRS) Centre Énergie Matériaux TélécommunicationsVarennes J3X 1P7Canada Department of Chemistry Indian Institute of Technology MandiHimachal PradeshIndia Department of Electrical Engineering École de Technologie SupérieureMontréal H3C 1K3Canada

Due to its fascinating and tunable optoelectronic properties,semiconductor nanomaterials are the best choices for multidisciplinary applications.Particularly,the use of semiconductor photocatalysts is one of the promising ways to harness solar energy for useful applications in the field of energy and environment.In recent years,metal oxide-based tailored semiconductor photocatalysts have extensively been used for photocatalytic conversion of carbon dioxide(CO_(2))into fuels and other useful products utilizing solar energy.This is very significant not only from renewable energy consumption but also from reducing global warming point of view.Such current research activities are promising for a better future of society.The present mini-review is focused on recent developments(2–3 years)in metal oxide semiconductor hybrid photocatalysts-based photo-electrochemical conversion of CO_(2)into fuels and other useful products.First,general mechanism of photo-electrochemical conversion of CO_(2)into fuels or other useful products has been discussed.Then,various metal oxide-based emerging hybrid photocatalysts including tailoring of their morphological,compositional,and optoelectronic properties have been discussed with emphasis on their role in enhancing photoelectrochemical efficienty.Afterwards,mechanism of their photo-electrochemical reactions and applications in CO_(2)conversion into fuels/other useful products have been discussed.Finally,challenges and future prospects have been discussed followed by a summary.

关键词： metal-oxide semiconductors nanohybrid photocatalysts photo-electrochemical CO_(2)conversion tailoring morphology fuels challenges and future prospects

Toward carbon neutrality by artificial photosynthesis

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Frontiers in Energy 2024年第1期18卷 54-55页

作者： Baowen ZHOU Minhua SHAO Sharif Md.SADAF shuhui sun Key Laboratory for Power Machinery and Engineering of the Ministry of Education Research Center of Renewable Synthetic FuelSchool of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemical and Biological Engineering Energy InstituteThe Hong Kong University of Science and TechnologyHong KongChina Institut National de la Recherche Scientifique(INRS)-CenterÉnergie Matériaux Télécommunications VarennesQuebec J3X 1P7Canada

CO_(2)is not only the primary cause of climate change but also an abundant and recyclable carbon resource.The breakthrough in emerging disruptive technologies such as carbon capture and storage(CCS),power-to-X,and direct air capture(DAC)is fundamental to achieving carbon neutrality.Among these technologies,artificial photosynthesis offers an attractive method for recycling carbon dioxide and water into fuels and chemicals using solar energy(CO_(2)+H_(2)O+sunlight→fuels+chemicals).It holds great promise for addressing the critical challenges associated with elevated CO_(2)concentrations and securing a sustainable supply of fuels and chemicals for economic sectors.

关键词： neutral holds breakthrough

Construction of MnS/MoS_(2) heterostructure on two-dimensional MoS_(2) surface to regulate the reaction pathways for high-performance Li-O_(2) batteries

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Journal of Energy Chemistry 2024年第6期93卷 443-452,I0012页

作者： Guoliang Zhang Han Yu Xia Li Xiuqi Zhang Chuanxin Hou shuhui sun Yong Du Zhanhu Guo Feng Dang Key Laboratory for Liquid-Solid Structure Evolution and.Processing of Materials(Ministry of Education) Shandong UniversityJinan 250061ShandongChina School of Environmental and Material Engineering Yantai UniversityYantai 264005ShandongChina Institute National de la Recherche Scientifique CentreÉnergie Matériaux et TélécommunicationsVarennesQuébec J31S2Canada State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083HunanChina Integrated Composites Lab Department of Mechanical and Construction EngineeringNorthumbria UniversityNewcastle Upon TyneNE18STUK

The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.

关键词： Li-O_(2)batteries Two-dimensional materials MnS/MoS_(2)heterostructure Edge plane Adsorption behavior

Identification of FOXO1 as a geroprotector in human synovium through single-nucleus transcriptomic profiling

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Protein & Cell 2024年第6期15卷 441-459页

作者： Feifei Liu Yi Lu Xuebao Wang shuhui sun Huize Pan Min Wang Zehua Wang Weiqi Zhang Shuai Ma Guoqiang sun Qun Chu Si Wang Jing Qu Guang-Hui Liu State Key Laboratory of Membrane Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China Sports Medicine Department Beijing Jishuitan HospitalCapital Medical UniversityBeijing 100035China State Key Laboratory of Stem Cell and Reproductive Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China University of Chinese Academy of Sciences Beijing 100049China Institute for Stem Cell and Regeneration Chinese Academy of SciencesBeijing 100101China Beijing Institute for Stem Cell and Regenerative Medicine Beijing 100101China National Laboratory of Biomacromolecules Institute of BiophysicsChinese Academy of SciencesBeijing 100101China Division of Life Sciences and Medicine School of Life SciencesUniversity of Science and Technology of ChinaHefei 230001China CAS Key Laboratory of Genomic and Precision Medicine Beijing Institute of GenomicsChinese Academy of Sciences and China National Center for BioinformationBeijing 100101China The Fifth People’s Hospital of Chongqing Chongqing 400062China Advanced Innovation Center for Human Brain Protection and National Clinical Research Center for Geriatric Disorders Xuanwu Hospital Capital Medical UniversityBeijing 100053China Aging Translational Medicine Center International Center for Aging and CancerBeijing Municipal Geriatric Medical Research CenterXuanwu HospitalCapital Medical UniversityBeijing 100053China

The synovium,a thin layer of tissue that is adjacent to the joints and secretes synovial fluid,undergoes changes in aging that contribute to intense shoulder pain and other joint diseases.However,the mechanism underlying human synovial aging remains poorly characterized.Here,we generated a comprehensive transcriptomic profile of synovial cells present in the subacromial synovium from young and aged individuals.By delineating aging-related transcriptomic changes across different cell types and their associated regulatory networks,we identified two subsets of mesenchymal stromal cells(MSCs)in human synovium,which are lining and sublining MSCs,and found that angiogenesis and fibrosis-associated genes were upregulated whereas genes associated with cell adhesion and cartilage development were downregulated in aged MSCs.Moreover,the specific cell-cell communications in aged synovium mirrors that of aging-related inflammation and tissue remodeling,including vascular hyperplasia and tissue fibrosis.In particular,we identified forkhead box O1(FOXO1)as one of the major regulons for aging differentially expressed genes(DEGs)in synovial MSCs,and validated its downregulation in both lining and sublining MSC populations of the aged synovium.In human FOXO1-depleted MSCs derived from human embryonic stem cells,we recapitulated the senescent phenotype observed in the subacromial synovium of aged donors.These data indicate an important role of FOXO1 in the regulation of human synovial aging.Overall,our study improves our understanding of synovial aging during joint degeneration,thereby informing the development of novel intervention strategies aimed at rejuvenating the aged joint.

关键词： FOXO1 degeneration inflammation

Lithium sulfide:a promising prelithiation agent for high-performance lithium-ion batteries

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SusMat 2024年第1期4卷 34-47页

作者： Junkang Huang Weifeng Li Wenli Zhang Bixia Lin Yang Wang SiuWing Or shuhui sun Zhenyu Xing School of Chemistry South China Normal UniversityGuangzhouP.R.China Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhouP.R.China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchunP.R.China Department of Electrical and Electronic Engineering The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong Institut National de la Recherche Scientifique(INRS) Centreénergie Matériaux TélécommunicationsVarennesCanada

Lithium-ion batteries are widely used in portable electronics and electric vehicles due to their high energy density,stable cycle life,and low self-discharge.However,irreversible lithium loss during the formation of the solid electrolyte interface greatly impairs energy density and cyclability.To compensate for the lithium loss,introducing an external lithium source,that is,a prelithiation agent,is an effective strategy to solve the above problems.Compared with other prelithiation strategies,cathode prelithiation is more cost-effective with simpler operation.Among various cathode prelithiation agents,we first systematically summarize the recent progress of Li_(2)S-based prelithiation agents,and then propose some novel strategies to tackle the current challenges.This review provides a comprehensive understanding of Li_(2)S-based prelithiation agents and new research directions in the future.

关键词： Li-ion batteries prelithiation Li2S prelithiation agent metallothermic reduction reaction

A single-nucleus transcriptomic atlas of primate liver aging uncovers the pro-senescence role of SREBP2 in hepatocytes

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Protein & Cell 2024年第2期15卷 98-120页

作者： Shanshan Yang Chengyu Liu Mengmeng Jiang Xiaoqian Liu Lingling Geng Yiyuan Zhang shuhui sun Kang Wang jian Yin Shuai Ma Si Wang Juan Carlos Izpisua Belmonte Weiqi Zhang Jing Qu Guang-Hui Liu Advanced Innovation Center for Human Brain Protection and National Clinical Research Center for Geriatric Disorders Xuanwu Hospital Capital Medical UniversityBeijing 100053China State Key Laboratory of Membrane Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China Aging Translational Medicine Center International Center for Aging and CancerBeijing Municipal Geriatric Medical Research CenterXuanwu HospitalCapital Medical UniversityBeijing 100053China State Key Laboratory of Stem Cell and Reproductive Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China CAS Key Laboratory of Genomic and Precision Medicine Beijing Institute of GenomicsChinese Academy of Sciences and China National Center for BioinformationBeijing 100101China Xuanwu Hospital Capital Medical University Beijing 100053China University of Chinese Academy of Sciences Beijing 100049China Institute for Stem Cell and Regeneration Chinese Academy of SciencesBeijing 100101China Beijing Institute for Stem Cell and Regenerative Medicine Beijing 100101China Aging Biomarker Consortium Beijing 100101China Altos Labs Inc.San DiegoCA 94022USA

Aging increases the risk ofliver diseases and systemic susceptibility to aging-related diseases.However,cell type-specific changes and the underlying mechanism of liver aging in higher vertebrates remain incompletely characterized.Here,we constructed the first single-nucleus transcriptomic landscape of primate liver aging,in which we resolved cell type-specific gene expression fluctuation in hepatocytes across three liver zonations and detected aberrant cell-cell interactions between hepatocytes and niche cells.Upon in-depth dissection of this rich dataset,we identifed impaired lipid metabolism and upregulation of chronic inflammation-related genes prominently associated with declined liver functions during aging.In particular,hyperactivated sterol regulatory element-binding protein(SREBP)signaling was a hallmark of the aged liver,and consequently,forced activation of SREBP2 in human primary hepatocytes recapitulated in vivo aging phenotypes,manifesting as impaired detoxification and accelerated cellular senescence.This study expands our knowledge of primate liver aging and informs the development of diagnostics and therapeutic interventions for liver aging and associated diseases.

关键词： single-nucleus RNA sequencing liver hepatocytes aging senescence SREBP2

CRL2^(APPBP2)-mediated TSPYL2 degradation counteracts human mesenchymal stem cell senescence

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Science China(Life Sciences) 2024年第3期67卷 460-474页

作者： Daoyuan Huang Qian Zhao Kuan Yang Jinghui Lei Ying Jing Hongyu Li Chen Zhang Shuai Ma shuhui sun Yusheng Cai Guibin Wang Jing Qu Weiqi Zhang Si Wang Guang-Hui Liu Advanced Innovation Centerfor Human Brain Protection National Clinical Research Centerfor Geriatric DisordersXuanwu Hospital Capital Medical UniversityBeijing 100053China State Key Laboratory of Stem Cell and Reproductive Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China Aging Translational MedicineCenter International Centerfor Aging and CancerBejing Municipal GeriatricMedical Research CenterXuanwu HospitalCapital Medical UniversityBeijing 100053China State Key Laboratory of Membrane Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China University of Chinese Academy of Sciences Beijing 100049China Beijing Institute for Stem Cell and Regenerative Medicine Beijing100101China CAS Key Laboratory of Genomic and Precision Medicine Bejing Institute of Genomics and China National Center for BioinformationChinese Academy of SciencesBeijing 100101China Institute for Stem Cell and Regeneration CASBeijing 100101China The Fifth People's Hospital of Chongqing Chongqing 400062China Sino-Danish Cllege University of Chinese Academy of SciencesBeijing101408China National Laboratory of Biomacromolecules CAS Center for Excelence in BiomacromoleculesInstitute of BiophysicsChinese Academy of SciencesBeijing100101China State Key Laboratory of Proteomics Beijing Proteome Research CenterNational Center for Protein Sciences(Beijing)Beijing Institute of LifeomicsBeijing 102206China

Cullin-RING E3 ubiquitin ligases(CRLs),the largest family of multi-subunit E3 ubiquitin ligases in eukaryotic cells,represent core cellular machinery for executing protein degradation and maintaining proteostasis.Here,we asked what roles Cullin proteins play in human mesenchymal stem cell(hMSC)homeostasis and senescence.To this end,we conducted a comparative aging phenotype analysis by individually knocking down Cullin members in three senescence models:replicative senescent hMSCs,Hutchinson-Gilford Progeria Syndrome hMSCs,and Werner syndrome hMSCs.Among all family members,we found that CUL2 deficiency rendered hMSCs the most susceptible to senescence.To investigate CUL2-specific underlying mechanisms,we then applied CRISPR/Cas9-mediated gene editing technology to generate CUL2-deficient human embryonic stem cells(hESCs).When we differentiated these into h MSCs,we found that CUL2 deletion markedly accelerates hMSC senescence.Importantly,we identified that CUL2 targets and promotes ubiquitin proteasome-mediated degradation of TSPYL2(a known negative regulator of proliferation)through the substrate receptor protein APPBP2,which in turn downregulates one of the canonical aging marker-P21^(waf1/cip1),and thereby delays senescence.Our work provides important insights into how CRL2^(APPBP2)-mediated TSPYL2 degradation counteracts hMSC senescence,providing a molecular basis for directing intervention strategies against aging and aging-related diseases.

关键词： Cullins stem cell senescence aging proteostasis ubiquitination APPBP2 TSPYL2

Multi-factor principle for electrolyte additive molecule design for facilitating the development of electrolyte chemistry

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Green Energy & Environment 2022年第1期7卷 1-2页

作者： shuhui sun Institut National de la Recherche Scientifique(INRS)-Center for Energy Materials and TelecommunicationsVarennesQuébec J3X 1S2Canada

When I read the paper“Electrolytes enriched by potassium perfluorinated sulfonates for lithium metal batteries”from Prof.Jianmin Ma’s group,which was published in Science Bulletin(***/10.1016/j.scib.2020.09.018),I felt excited as presented a multi-factor principle for applying potassium perfluorinated sulfonates to suppress the dendrite growth and protect the cathode from the viewpoint of electrolyte additives.The effects of these additives are revealed through experimental results,molecular dynamics simulations and first-principle calculations.Specifically,it involves the influence of additives on Li^(+)solvation structure,solid electrolyte interphase(SEI),Li growth and nucleation.Following the guidance of the multi-factor principle,every part of the additive molecule should be utilized to regulate electrolytes.This multifactor principle for electrolyte additive molecule design(EAMD)offers a unique insight on understanding the electrochemical behavior of iontype electrolyte additives on both the Li metal anode and high-voltage cathode.In these regards,I would be delighted to write a highlight for this innovative work and,hopefully,it may raise more interest in the areas of electrolyte additives.

关键词： Lithium metal batteries Multi-factor principle Electrolyte additives Dendrite growth suppression Lithium protection