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Rare Metals 2024年第2期43卷 588-598页

作者： Fei Wang Han Gao Zhao-Yu Niu Yao-Peng Zheng Ming-Yan Chuai Jia-Nan Xu State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China

In the current situation where the practical application of silicon anode materials encounters great challenges,silicon oxide(SiO_(x),0≤x≤2)has attracted the attention of researchers due to its relatively small volume expansion,stable cycling performance,and low cost,which is possible to realize commercial applications earlier than silicon ***,it remains a challenge to prepare SiO_(x)materials with long-term stable cycling performance and high Coulombic efficiency using low-cost *** this work,SiO_(x)anode material with high Coulombic efficiency and good long-term cycling stability was prepared at a low cost by hydrolysis of siloxane and in situ polymerization of phenolic *** hydrolysis of siloxane was further regulated by different silane coupling agents to regulate the size and microstructure of prepared SiO_(x)materials,which displayed the substantially improved electrochemical *** excellent electrochemical performance of SiO_(x)prepared by regulated hydrolysis of siloxane with silane coupling agents is attributed to the effect of silane coupling agent on size and microstructure of SiO_(x),revealing that the strategy of modulating the hydrolysis of siloxane by silane coupling agent is a potential method to prepare high-performance SiO_(x)materials.

关键词： Hydrolysis Silane coupling agent Long cycle SiO_(x) anode Lithium-ion battery(LIB)

Atomic-level coupled RuO_(2)/BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction

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Journal of Energy chemistry 2024年第1期88卷 356-362,I0009页

作者： Yueying Yan Tian Meng Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of *** this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of *** RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water *** research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.

关键词： Heterostructure Hydrogen evolution reaction Interfacial electron transfer Oxygen vacancies

Exploring the potential of constructing a hybrid supercapacitor with FeCoNi-LDH porous material containing oxygen vacancies for high-performance energy storage applications

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Nano Research 2024年第9期17卷 8134-8144页

作者： Jihao Su Ling Yang Dengbin Yu Shaojun Dong State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China College of chemistry Jilin UniversityChangchun 130022China University of Science and Technology of China Hefei 230026China

A significant challenge in developing high-performance hybrid supercapacitors(HSCs)is the need to reasonably construct advanced architectures that consist of various components and exhibit superior electrochemical capacitance *** FeCoNi-layered double hydroxide(FeCoNi-LDH)porous material has a specific capacitance of 1960 F·g^(-1)when used as the anode material at 1 A·g^(-1).The FeCoNi-LDH material exhibits nanoplates with a distinct spindle morphology on their *** to the combined action of the three metals and abundant oxygen vacancies,they exhibit unique rate performance and cycle *** electronic structure of LDH and the regulation of oxygen vacancy were confirmed by density functional theory(DFT)*** suggests that the strength of hydroxide can reduce the energy required for oxygen vacancy formation in FeCoNi-LDH nanosheets and enhance ion and charge transfer,as well as electrolyte adsorption on the electrode *** FeCoNi-LDH//activated carbon(AC)HSC has an energy density of 53.2 Wh·kg^(-1)at a power density of 800 W·kg^(-1),surpassing other devices composed of comparable materials during the same *** study made significant advances in the design and synthesis of a ternary LDH porous structure with distinct oxygen vacancies,as well as its potential application in electrochemical energy storage.

关键词： oxygen vacancy FeCoNi-layered double hydroxide(FeCoNi-LDH) theory calculation electrode material hybrid supercapacitor

Vacancy engineering induced reaction kinetics enhancement of cobalt metaphosphate for pH-universal hydrogen evolution

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Nano Research 2024年第5期17卷 3879-3887页

作者： Yuting Chen Tian Meng Zhicai Xing Yueying Yan Yang Yang Bohan Yao Dewen Wang Xiurong Yang State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Developing efficient pH-universal hydrogen evolution reaction(HER)catalysts is critical in the field of water electrolysis,however,which is severely hampered by the sluggish kinetics in alkaline ***,a ruthenium(Ru)incorporation induced vacancy engineering strategy is firstly proposed to precisely construct oxygen vacancy(V_(O))-riched cobalt-ruthenium metaphosphate(CRPO)for high-efficiency pH-universal *** V_(O) modifies the electronic structure,improves the superficial hydrophilic and gas spillover capacity,it also reduces the coordination number of Ru atoms and regulates the coordination *** calculations indicate that Ru tends to adsorb H_(2)O and H^(*),whereas V_(O) tends to adsorb OH^(-),which greatly promotes the H_(2)O adsorption and the dissociation of HO-H ***,CRPO-2 exhibits remarkable HER performance,the mass activity is about 18.34,21.73,and 38.07 times higher than that of Pt/C in acidic,neutral,and alkaline media,respectively,at the same time maintain excellent *** findings may pave a new avenue for the rational design of electrocatalysts toward pH-universal water electrolysis.

关键词： cobalt metaphosphate pH-universal hydrogen evolution reaction(HER) vacancy engineering low-coordination atoms oxygen vacancy

In-situ UV-Vis Spectroscopy of Trisulfur Radicals in Lithium-Sulfur Batteries

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Chemical Research in Chinese Universities 2024年第2期40卷 279-286页

作者： DOU Renju WANG Qin REN Xiaoyan LU Lehui School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei230026P.R.China State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022P.R.China

Here we employ in-situ UV-Vis spectroscopy to monitor the sulfur redox reaction with oxygen-containing molecules as an additive,for example,biphenyl-4,4′-dicarboxylic acid(BDC).Furthermore,Raman spectrum,electron paramagnetic resonance(EPR),and electrospray ionization-mass spectrometry(ESI-MS)measurements reveal that the formation of BDC-S_(3)•^(‒)complexes can establish the long-term stability of polysulfide radicals,change the kinetics of sulfur redox reaction,and then generate decent capacity retention and rate *** to the density functional theory(DFT)analysis,S_(3)•^(‒)radicals are the underlying product of S_(6)^(2‒)cleavage,owing to the decreased chemical energy and the increased stability of S_(3)•^(‒)radicals through Lewis acid-base *** assembled Li-S batteries with BDC additive deliver a high reversible capacity of 420 mA·h·g^(−1)over 200 cycles with over 98%Coulombic efficiency,under the current density of 0.2 C.

关键词： Radical Polysulfide In-situ UV-Vis Spectroscopy Electrolyte additive Lithium-sulfur battery

Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key lab.ratory of electroanalytical chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

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 lab.ratory of electroanalytical chemistry and Jilin Province Key lab.ratory 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 lab.ratory 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 *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** 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 *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** 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 *** 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 *** 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

A Highly Efficient Ni/Al_(2)O_(3)-LaO_(x) Catalyst for the Reductive Amination of Furfural to Furfurylamine:the Promoting Effect of La

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Chemical Research in Chinese Universities 2024年第1期40卷 36-46页

作者： YANG Yinze ZHANG Liyan ZHOU Leilei CHENG Haiyang ZHAO Fengyu State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied chemistry and Engineering University of Science Technology of ChinaHefei 230026P.R.China Jilin Province Key lab.ratory of Green chemistry and Process Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China

The reductive amination of furfural to furfurylamine is an important and still challenging topic in the field of biomass conversion. In this work, we prepared a series of Ni/Al_(2)O_(3)-LaO_(x) catalysts by co-precipitation method, the role of La played in promoting the catalytic performances of reductive amination furfural was discussed based on the changes in the electronic state of Ni species, acidity, and Ni particle size. The catalytic activity and the selectivity of furfurylamine are highly dependent on the surface properties and the structure of the catalyst. The addition of La promoted the amount of strong acidic sites and the H2dissociation and spillover on the surface, thus inducing the improvement of the catalytic activity and furfurylamine selectivity. The Ni/Al_(2)O_(3)-0.5LaO_(x)catalyst with suitable acid sites gave a high yield of furfurylamine (94.9%) under mild reaction conditions. Moreover, the catalyst could be recycled five times without significant loss in activity. The Ni/Al_(2)O_(3)-LaO_(x) catalyst is of great promise in the production of amines via reductive amination reaction.

关键词： Reductive amination Furfural Nickel catalyst Furfurylamine Lanthanum

Aggregation-induced T_(1)/T_(2) contrast enhancement for magnetic resonance imaging-guided intraoperative surgery

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Science China chemistry 2024年第6期67卷 2046-2055页

作者： Wenbo Sun Bin Yu Dianshuai Huang Chunhuan Jiang Wei Wang Jianhua Liu Zonghua Wang Lehui Lu State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China College of chemistry and Chemical Engineering Shandong Sino-Japanese Center for Collaborative Research of Carbon NanomaterialsQingdao Application Technology Innovation Center of Photoelectric Biosensing for Clinical Diagnosis and TreatmentQingdao UniversityQingdao266071China Department of Radiology Second Hospital of Jilin UniversityChangchun130041China

Magnetic resonance imaging(MRI)plays an important role in precision medicine that is hampered by the lack of contrast agents with high efficiency and the ability to translate diagnostic accuracy into therapeutic ***,we demonstrate a DNA-based MRI probe that overcomes previous single-mode enhancement and provides a mechanism of action for aggregationinduced dual-modal MRI signal enhancement.A facile method is developed to produce aggregated T_(1)/T_(2)dual-modal NaGdF_(4):Dy@PDA-DNA(PDA=polydopamine)MRI *** aggregated,this probe can further amplify MRI signal intensity and exhibit improved geometrical and positional stability in *** performance of the NaGdF_(4):Dy@PDA-DNA MRI probe toward MRI-guided preoperative planning and visualization-guided surgery is verified using an orthotopic tumor-bearing mouse *** result shows that the rapid metabolism of the degraded probe leads to the mitigation of long-term toxic ***,the developed high-performance MRI probe is of great significance for enhancing MRI diagnostic accuracy into precision medical therapeutic interventions.

关键词： MRI probe DNA aggregation-induced T_(1)/T_(2)contrast enhancement precision medicine degradable probe

Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing State Key lab.ratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China lab.ratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key lab.ratory of Low Carbon Chemical Power Sources Changchun 130022China State Key lab.ratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.