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Confined Mn^(2+) enables effective aerobic oxidation catalysis

Science China chemistry 2024年第5期67卷 1545-1553页

作者： Desheng Yuan Sicong Ma Xiao Kong Chi Zhang Lin Chen Chengsheng Yang Lihua Wang Zhen Liu Lin Ye Yongmei Liu Rui Ma Zhi-Pan Liu Yifeng Zhu Yong Cao Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China Department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key Laboratory of Synthetic and Self-Assembly chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key Laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but challenging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

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Synthesis of straight-chain C_(49)H_(100) alkane using a modular splicing strategy

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Journal of energy chemistry 2024年第5期92卷 414-421页

作者： Bing Ma Jingqing Tian Xueling Lang Shutao Lei Bolong Li Chen Zhao Shanghai Key Laboratory of Green chemistry and Chemical processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China School of Materials Science and Engineering Nankai UniversityTianjin 300350China

Ultra-long n-alkanes are highly valuable in both scientific research and as major constituents of specialty high-melting-point *** conventional methods(e.g.,Fischer–Tropsch(FT),ethylene oligomerization,and polyethylene cracking)typically resulting in wide n-alkane distributions,the elaborate design strategy presented herein allows the direct synthesis of pure,long n-alkanes using a modular splicing method with acetone,furfural,and fatty acid anhydrides or acyl chlorides as *** herein approach is based on a simple four-step catalytic reaction scheme involving C–C chain elongation and C–O bond *** synthesized pure n-alkanes had a carbon chain length as high as C_(49)(total yield of 49%).The synthesis approach also allows to selectively prepare n-alkanes with even and odd carbon numbers ranging from C15 to C_(49).This process represents a great breakthrough in the synthesis of long-chain pure n-alkanes,surpassing the carbon number limitations reported in previous methodologies.

关键词： Straight-chain alkane Aldol condensation F-Cacylation Hydrodeoxygenation

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Multifunctional photon conversion materials for enhancing silicon solar cells

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Light(Science & Applications) 2024年第4期13卷 598-601页

作者： Yiyan Zhang Guanying Chen MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of Technology150001 HarbinChina

A type of multifunctional erbium(Er^(3+))and ytterbium(Yb^(3+))codoped NaY(WO4)2 phosphors,with simultaneous photon upconversion,photon quantum cutting,and luminescence ratiometric temperature sensing abilities,have b... 详细信息

关键词： photon luminescence quantum

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The dynamic catalysis of Ga/ZSM-5 catalysts for propane-CO2 coupling conversion to aromatics and syngas

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Journal of energy chemistry 2024年第10期97卷 513-519页

作者： Yonggui Song Zhong-Pan Hu Haohao Feng Enze Chen Le Lv Yimo Wu Zhen Liu Yong Jiang Xiaozhi Su Feifei Xu Mingchang Zhu Jingfeng Han Yingxu Wei Svetlana Mintova Zhongmin Liu The Key Laboratory of the Inorganic Molecule-Based chemistry of Liaoning Province and Laboratory of Coordination chemistry Shenyang University of Chemical Technology National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Shanghai Advanced Research institute Chinese Academy of Sciences Normandie University Laboratory of Catalysis and Spectrochemistry (LCS) ENSICAENUNICAEN CNRS

Alkane coupling with CO2by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO2are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO2hydrogenation,reverse water-gas shift reaction,and propane-CO2coupling ***,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO2during the propane and CO2coupling *** optimizing the reaction conditions,a notable propane conversion rate of 97.9% and an impressive aromatics selectivity of 80.6% in hydrocarbons can be achieved at the conditions of 550℃ and CO2/C3H8of 4.13CO2isotope experiments illustrate that C-atoms of CO2can enter into CO（86.5%） and aromatics（10.8%）during the propane-CO2coupling reaction *** situ XANES and FTIR spectroscopies at 550℃and H2/C3H8atmosphere reveal that GaOxspecies can be gradually dispersed into [GaH2]+/[GaH]2+on the Bronsted acid sites of ZSM-5 zeolite during H2and/or C3H8treatment,which are the real active sites for propane-CO2coupling *** situ CO2-FTIR experiments demonstrate that the [GaH2]+/[GaH]2+species can react with CO2and accelerate the propane and CO2coupling *** work not only presents a cost-effective avenue for CO2utilization,but also contributes to the active site design for improved alkane and CO2activation in coupling reaction system.

关键词： Carbon dioxide Ga/ZSM-5 Gallium hydride Propane aromatization Spectroscopy

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Mechanism of high Li-ion conductivity in poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network based electrolyte revealed by solid-state NMR

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Journal of energy chemistry 2024年第6期93卷 377-383,I0010页

作者： Fan Li Tiantian Dong Yi Ji Lixin Liang Kuizhi Chen Huanrui Zhang Guanglei Cui Guangjin Hou State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Qingdao Industrial energy Storage Research institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101ShandongChina

Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid ***-linked polymers have the potential to further improve the mechanical property without trading off Li-ion *** this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion *** utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion *** is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio *** such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.

关键词： ssNMR Lithium-ion mobility Cross-link Solid polymer electrolyte

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Tuning the Surface Field by Embedding Cations into Metals to Direct the Reaction Pathway of CO_(2) Electroreduction

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CCS chemistry 2024年第3期6卷 631-640页

作者： Pei Zhang Meng Zhou Shiqiang Liu Xueqing Xing Jiahao Yang Peng Chen Yaoyu Yin Yingying Cheng Xing Tong Jun Ma Qinggong Zhu Xiaofu Sun ZhongJun Chen Xinchen Kang Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green chemistry and Chemical processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 School of chemistry University of Chinese Academy of SciencesBeijing 100049

The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is ***,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant *** to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of *** the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway *** a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.

关键词： CO_(2)electroreduction tuneable products electrical field reaction pathway cations embedding

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Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery

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Rare Metals 2024年第3期43卷 1006-1016页

作者： Xin-Yang Chen Xue-Jie Gao Han-Yan Wu Yu-Long Liu Xiao-Fei Yang Run-Cang Sun Center for Lignocellulosic chemistry and Biomaterials College of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian116034China Division of energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China School of chemistry Northeast Normal UniversityChangchun130024China

Quasi-solid-state lithium metal batteries(QSSLMBs)assembled with polyvinylidene fluoride(PVDF)are a promising class of next-generation rechargeable batteries due to their safety,high energy density,and superior interfacial ***,PVDF has a series of inherent drawbacks such as low ionic conductivity,ease of crystallization,and hydrophobic character that leading to poor cell *** tackle these issues,a lignin-reinforced PVDF electrolyte is proposed in this work to solve these drawbacks of PVDF and enhance the comprehensive performance of *** lithophilic polar groups of lignin can promote uniform deposition of Li on the *** with the improved mechanical properties can efficiently prevent Li dendrites penetration through the *** addition,more active sites provided by lignin can also enhance Li^(+)transport and lead to a faster electrochemical reaction *** from the ingenious design,Li symmetric cells with 5%lignin-PVDF quasi-solid-state electrolyte can operate for 900 h at a high current density/capacity of 5 mA·cm^(-2)/5 mAh·cm^(-2),while shortcircuiting occurs after 56 h for the counterpart(pure PVDF).Moreover,a full cell of Li/5%lignin-PVDF/LFP cell demonstrates a high capacity of 96.2 mAh·g^(-1)after 2000 cycles at 10 *** work is expected to open up promising opportunities to develop other high-energy/power-density QSSLMBs.

关键词： Quasi-solid-state electrolyte Lignin PVDF Dendrite-free Li metal battery

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Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu Department of Applied chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen *** extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still ***,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox *** entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction *** a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts *** encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

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Photothermal catalysts for efficient and clean fuel production at atmospheric pressure

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Science China chemistry 2024年第6期67卷 1762-1764页

作者： Xinwei Guan Yang Chen Tianyi Ma School of Science RMIT UniversityMelbourneVIC3000Australia institute of Clean energy chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang110036China

The use of waste carbon resources to produce valuable chemicals and hydrocarbon fuels has attracted great interest in recent *** a transformation not only maximises the utilisation of carbon resources but also plays a... 详细信息

关键词： thermal transformation clean

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Hard carbon for sodium storage:Mechanism and performance optimization

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Nano Research 2024年第7期17卷 6038-6057页

作者： Yongxin Wang Meng Li Yu Zhang Naiqing Zhang State Key Laboratory of Urban Water Resource and Environment School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China School of energy Science and Engineering Harbin Institute of TechnologyHarbin 150001China

Due to the shortage of lithium resource reserves and the pressure of rising prices,sodium-ion batteries have regained the attention of the public,and shown great potential for application in the fields of grid energy storage and low-speed vehicles to achieve the purpose of complementing lithium-ion batteries,so it is imperative to promote the commercial application of sodiumion *** sodium-ion battery anode materials,hard carbon is the material most likely to be used ***,there is still much work to be done before its *** review provides a comprehensive overview of the current research status from the following three ***,the microstructure and sodium storage active sites of hard carbon are ***,the mechanism of sodium storage in hard carbon is investigated,which can be broadly categorized into four model,“insertion–filling”,“adsorption–insertion”,“adsorption–filling”,and“multistage”.Finally,from the perspective of improving the electrochemical performance of hard carbon,the performance improvement strategies proposed in recent years are *** with the performance of hard carbon commercial products of some enterprises,the future development goal of hard carbon is prospected,hoping that all sectors of society can work hard for this common goal.

关键词： sodium-ion battery hard carbon mechanism performance optimization

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