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Unraveling the Fundamental Mechanism of Interface Conductive Network Influence on the Fast‑Charging Performance of SiO‑Based Anode for Lithium‑Ion Batteries

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Nano-Micro Letters 2024年第3期16卷 53-68页

作者： Ruirui Zhang Zhexi Xiao Zhenkang Lin Xinghao Yan Ziying He Hairong Jiang Zhou Yang Xilai Jia Fei Wei beijing key laboratory of green chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China beijing key laboratory of chemical power source and green catalysis School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Institute of Polymer Science and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China

Progress in the fast charging of high-capacity silicon monoxide(SiO)-based anode is currently hindered by insufficient conductivity and notable volume expansion.The construction of an interface conductive network effectively addresses the aforementioned problems;however,the impact of its quality on lithium-ion transfer and structure durability is yet to be explored.Herein,the influence of an interface conductive network on ionic transport and mechanical stability under fast charging is explored for the first time.2D modeling simulation and Cryo-transmission electron microscopy precisely reveal the mitigation of interface polarization owing to a higher fraction of conductive inorganic species formation in bilayer solid electrolyte interphase is mainly responsible for a linear decrease in ionic diffusion energy barrier.Furthermore,atomic force microscopy and Raman shift exhibit substantial stress dissipation generated by a complete conductive network,which is critical to the linear reduction of electrode residual stress.This study provides insights into the rational design of optimized interface SiO-based anodes with reinforced fast-charging performance.

关键词： Fast charging SiO anode Interface conductive network Ionic transport Mechanical stability

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Enhancing green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma key laboratory for green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State key laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of chemical Engineering The University of AdelaideAdelaideSA 5005Australia State key laboratory of High‑Efficiency Utilization of Coal and green chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial key laboratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关键词： green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid

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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang key laboratory of catalysis and Energy Materials Chemistry of Ministry of Education&Hubei key laboratory of catalysis and Materials Science South-Central Minzu UniversityWuhan 430074China Hubei key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique structures.The structural sensitivity of these catalysts is closely linked to their particle size and crystal form.Consequently,comprehending the structure–activity relationship requires the development of well-defined Co-based catalysts.Herein,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon nanospheres.The nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO nanoparticles.By adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal forms.The influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been investigated.The result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 nm.However,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(<7.7 nm).Significantly,when metallic fcc-Co^(0) particle size was reduced from 17.6 to 7.7 nm,the cobalt time yield increased to 6.7μmolCO·gCo^(-1)·s^(-1),indicating improved catalytic activity.At the same time,the CH_(4) selectivity decreased to 4.9%,suggesting a higher preference for hydrocarbon production.These findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch synthesis.The use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

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Palladium-catalyzed multi components oxy-aminofluorination and aminofluorination of gem-difluoroalkenes

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Chinese chemical Letters 2024年第2期35卷 420-425页

作者： Fen Wu Xin Li Junbiao Chang Dachang Bai State key laboratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative DrugKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringPingyuan LaboratoryHenan Normal UniversityXinxiang 453007China State key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Organofluorine compounds are widely used in the realm of drug discovery and material science.Herein,we developed palladium catalyzed intermolecular aminofluorination and oxy-aminofluorination of gem‑difluoroalkenes with N-fluorobenzenesulfonimide(NFSI),in which NFSI was used as the nitrogen source and oxidant.The reaction provides an efficient and straightforward synthesis route of a series ofα-trifluoromethyl benzylic amines.Notably,three/four components oxy-aminofluorination processes were realized to giveα-trifluoromethyl benzylic ether with a terminal amino group,which proceed through C(sp^(3))-O bond cleavage of easily available ether and simultaneous introduced a fluorine,an amino and an oxy substituent in one pot with excellent regioselectivity.The divergent reactivity not only included the incorporation of one ether molecular,but also much more challenged two ether insertion with excellent selectivity through succession C(sp^(3))-O bonds cleavage.This protocol allows for concise synthesis of high value amines with fluoroalkyl-substituents and selectively transformation of easily available ethers by high-valent palladium catalysis.

关键词： Palladium Multi components Aminofluorination Oxy-aminofluorination C(sp^(3))-O bond cleavage

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Selective photosynthesis of imines from biomass-derived aldehydes over Ni/TiO_(2)

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Rare Metals 2024年第3期43卷 1116-1124页

作者： Wu-Lin Li Qing-Qing Zhang Lin Dong Wen-Jun Zhang Li-Li Lin Zu-Peng Chen Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing210037China Institute of Industrial catalysis State Key Laboratory of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

Photocatalytic reductive amination of biomass-derived aldehydes is a desirable way to selectively upgrade biomass into value-added nitrogen-containing chemicals under mild conditions.However,it is challenging to produce imines in high selectivity because of the undesirable side reactions caused by the activity of functional groups.Here,we demonstrate the highly reactive and selective production of imines from biomass derived aldehydes via the photocatalytic reductive amination,using a defective TiO_(2)supported nickel catalyst.The employment of methanol as the hydrogen donor and ammonia solution as the nitrogen source avoids the use of high-pressure H_(2)and expensive amines,rendering the current catalytic process safe,economical,and environmentally friendly.In depth investigations attribute the improved separation and transfer of photogenerated charge carriers to the presence of oxygen vacancies and decorated Ni nanoparticles,thereby accelerating the production of imines from benzaldehyde amination(conversion,95.8%;seleetivity,95.2%).Furthermore,the developed system could be easily translated to the photocatalytic conversions of various biomass derived aldehydes,which provided an example of a cost-effective and sustainable approach for the valorization of biomass derived feedstocks.

关键词： Photocatalysis Biomass derivatives Imines Reduction amination Heterogeneous catalyst

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Reducing the voltage loss of Y-series acceptor based organic solar cells via ternary/quaternary strategies

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Chinese chemical Letters 2024年第2期35卷 70-86页

作者： Pengyu Zhang Zhiyang Zhang Heng Sun Jie Li Yi Chen Jiang Wang Chuanlang Zhan key laboratory of Advanced Materials Chemistry and Devices (AMC&DLab) of the Department of Education of Inner Mongolia Autonomous Region Inner Mongolia Key Laboratory of Green CatalysisCollege of Chemistry and Environment ScienceInner Mongolia Normal UniversityHuhehot 010022China

In recent years, with the emergence of non-fullerene fused-ring acceptors, power conversion efficiencies (PCEs) of organic solar cells (OSCs) have exceeded 19%.However, compared to inorganic or perovskite photovoltaic cells, a higher voltage loss has become one of the key factors limiting further improvement in the PCEs of OSCs.The ternary/quaternary strategy has been identified as a feasible and effective way to obtain high-efficiency OSCs.In this review, a brief outline is given of the key roles that guest materials played in reducing voltage losses in solar cell devices and a brief look at the future material design and the design of ternary/quaternary systems.

关键词： Organic solar cell Ternary/quaternary strategy Open-circuit voltage Voltage loss Non-radiative recombination loss

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Realizing methanol synthesis from CO and water via the synergistic effect of Cu^(0)/Cu^(+)over Cu/ZrO_(2) catalyst

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Journal of Energy Chemistry 2024年第6期93卷 126-134,I0004页

作者： Yuan Fang Fan Wang Yang Chen Qian Lv Kun Jiang Hua Yang Huibo Zhao Peng Wang Yuyan Gan Lizhi Wu Yu Tang Xinhua Gao Li Tan Institute of Molecular catalysis and In Situ/Operando Studies Fujian Key Laboratory of Electrochemical Energy Storage MaterialsState Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108FujianChina Leibniz-Institut für Katalyse e.V.an der Universität Rostock Albert-Einstein Strasse 9118059 RostockGermany Department of Chemistry Tsinghua UniversityBeijing 100084China State key laboratory of High-Efficiency Utilization of Coal and green chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021Ningxi1China

The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic state.The Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the reaction.Moreover,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic system.The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.

关键词： H_(2)O CO Methanol Cu-based catalysts t-ZrO_(2)

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Asymmetrically coordinated single atom Cu catalyst with unsaturated C-Cu-N structure for CO_(2) reduction to CO

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Nano Research 2024年第5期17卷 3911-3918页

作者： Zheng Liu Yuxuan Liu Jingqiao Zhang Ting Cao Zhiyi Sun Juzhe Liu Huishan Shang State key laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China SEPA key laboratory of Eco-Industry Chinese Research Academy of Environmental SciencesBeijing 100012China The key laboratory of Resources and Environmental System Optimization Ministry of EducationCollege of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China School of chemical Engineering Zhengzhou UniversityZhengzhou 450001China

Single atom catalysts(SACs)play a crucial role in energy catalysis due to their distinct coordination environment and high atomic utilization efficiency.This study focuses on the synthesis of a monatomic Cu catalyst with Cu-N1C1 coordination anchored to N-doped Ti_(3)C_(2)T_(x) MXene(Cu SA@N-Ti_(3)C_(2)T_(x))to achieve efficient reduction of CO_(2) to CO.Detailed characterization,including morphology and multispectral analysis,confirmed the uniform distribution of asymmetrically coordinated Cu atoms in unsaturated C-Cu-N bridge fragments on Ti_(3)C_(2)T_(x).The Cu SA@N-Ti_(3)C_(2)T_(x) catalyst exhibited an excellent CO selectivity with Faraday efficiency of 97.4%at-0.58 V vs.reversible hydrogen electrode(RHE)and satisfactory durability.The in situ X-ray absorption fine structure(XAFS)results confirmed that the carbon dioxide reduction reaction(CO_(2)RR)product distribution is mainly affected by potential-dependent valence change of Cu species.These findings highlight the extensive potential of tuning coordination structure of MXene-based single-atom catalysts for CO_(2) reduction reactions.

关键词： cooper single atom atomic regulation MXene Ti_(3)C_(2)T_(x) CO_(2)reduction

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Molecule aging induced by electron attacking

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Journal of Energy Chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State key laboratory of Electroanalytical Chemistry and Jilin Province key laboratory of Low Carbon chemical power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai key laboratory of Molecular catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

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Recent progress in photocatalytic NAD(P)H regeneration for photocatalytic-enzymatic-coupling system

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Frontiers of chemical Science and Engineering 2024年第4期18卷 1-24页

作者： Wei Lan Maodi Wang Huicong Dai Qihua Yang key laboratory of the Ministry of Education for Advanced catalysis Materials Zhejiang Key Laboratory for Reactive Chemistry on Solid SurfacesInstitute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

The enzymatic redox reactions in natural photosynthesis rely much on the participation of cofactors,with reduced nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate(NADH/NADPH)or their oxidized form(NAD+/NADP+)as an important redox power.The photocatalytic regeneration of expensive and unstable NADH/NADPH in vitro is an important process in enzymatic reduction and has attracted much research attention.Though different types of photocatalysts have been developed for photocatalytic NADH/NADPH regeneration,the efficiency is still relatively low.To elucidate the key factors affecting the performance of photocatalytic NADH/NADPH regeneration is helpful to rationally design the photocatalyst and improve the photocatalytic efficiency.In this paper,we overview the recent progress in photocatalytic NADH/NADPH regeneration with the focus on the strategies to improve the visible light adsorption,the charge separation and migration efficiency,as well as the surface reaction,which jointly determine the overall photocatalytic regeneration efficiency.The potential development of photocatalytic NADH/NADPH regeneration and photocatalyticenzymatic-coupling system is prospected finally.

关键词： photocatalytic-enzymatic coupling NAD(P)H regeneration photocatalysis efficiency

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