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The Mechanism of Water Oxidation from Mn-Based Heterogeneous Electrocatalysts

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Chinese Journal of Structural Chemistry 2022年第4期41卷 22-33页

作者： Shujiao Yang Lingshuang Qin Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119China

Searching for a renewable energy system is always the goal to fulfill sustainable development for the *** oxidation is considered as a crucial reaction to attain sustainable energy *** by the biological Mn_(4)CaO_(5)cluster,considerable effort has been devoted to developing highly efficient Mn-based heterogeneous catalysts and exploring intrinsic mechanism for water *** review begins with describing the structural characteristics of the Mn_(4)Ca O_(5)cluster and the proposed catalytic ***,the structural characteristics of synthetic Mn-based heterogeneous catalyst are summarized,with emphasis on the understanding of reaction mechanisms and the rate-determining ***,the strategy of understanding the catalytic mechanism of Mn-based water oxidation is prospected.

关键词： water oxidation Mn-based electrocatalysts oxygen evolution reaction structure mechanism

Highly efficient electrocatalytic nitrogen fixation enabled by the bridging effect of Ru in plasmonic nanoparticles

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Nano research 2023年第1期16卷 360-370页

作者： Hang Yin Jinwu Hu Caihong Fang Yuyang Wang Lixia Ma Nan Zhang Shouren Zhang Ruibin Jiang Jianfang Wang shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China College of Chemistry and Materials Science The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCenter for Nano Science and TechnologyKey Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesAnhui Normal UniversityWuhu 241000China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nanostructured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou 450006China Department of Physics The Chinese University of Hong KongHong Kong 999077China

Plasmon-generated hot electrons show great potential for driving chemical *** utilization efficiency of hot electrons is highly dependent on the interaction of the electronic states at the interfaces between plasmonic nanoparticles and other materials/*** interaction can produce new hybridized electron states,which permit direct hot-electron transfer,a more efficient transfer ***,Au usually has very weak interaction with most molecules because of its inertness,which makes direct hot-electron transfer ***,the improvement of the hot-electron transfer efficiency from Au to N_(2)is demonstrated by introducing a Ru bridging *** the N_(2)fixation rate and Faradic efficiency(FE)are enhanced by the excitation of *** enhancement of the N_(2)fixation rate is found to arise from plasmon-generated hot *** calculations show that the strong interaction of the Ru electronic states with the N_(2)molecular orbitals produces new hybridized electronic states,and the Ru d electrons also strongly couple with the Au sp *** a bridging role of Ru makes direct hot-electron transfer from Au to N_(2)possible,improving the FE of nitrogen *** findings demonstrate a new approach to increasing the utilization efficiency of plasmonic hot electrons for chemical reactions and will be helpful to the design of plasmonic catalysts in the future.

关键词： electrocatalytic nitrogen fixation Au/Ru electrocatalysts localized surface plasmon resonance electronic state hybridization hot electron

Direct Vibrational Energy Transfer in Monomeric Water Probed with Ultrafast Two Dimensional Infrared Spectroscopy

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Chinese Journal of Chemical Physics 2017年第6期30卷 619-625,I0001页

作者：周德霞魏千顺边红涛郑俊荣陕西师范大学化学化工学院应用表面与胶体化学教育部重点实验室西安710119 北京大学化学与分子工程学院北京分子科学国家实验室北京100871

Vibrational relaxation dynamics of monomeric water molecule dissolved in d-chloroform solution were revisited using the two dimensional Infrared （2D IR） spectroscopy. The vibrational lifetime of OH bending in monomeric water shows a bi-exponential decay. The fast compo- nent （T1=（1.2±0.1） ps） is caused by the rapid population equilibration between the vibrational modes of the monomeric water molecule. The slow component （T2=（26.4±0.2） ps） is mainly caused by the vibrational population decay of OH bending mode. The reorientation of the OH bending in monomeric water is determined with a time constant of t=（1.2±0.1） ps which is much faster than the rotational dynamics of water molecules in the bulk solution. Furthermore, we are able to reveal the direct vibrational energy transfer from OH stretching to OH bending in monomeric water dissolved in d-chloroform for the first time. The vibrational coupling and relative orientation of transition dipole moment between OH bending and stretching that effect their intra-molecular vibrational energy transfer rates are discussed in detail.

关键词： Vibrational energy transfer Confined water Ultrafast Infrared spectroscopy Monomeric water

Comparing electrocatalytic hydrogen and oxygen evolution activities of first-row transition metal complexes with similar coordination environments

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Journal of Energy Chemistry 2021年第12期30卷 659-666,I0016页

作者： Xiaotong Jin Xialiang Li Haitao Lei Kai Guo Bin Lv Hongbo Guo Dandan Chen Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119ShaanxiChina

Developing cheap and efficient electrocatalysts for water splitting is required for energy conversion *** first-row transition metal complexes have been shown to be active for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Metal ions play crucial roles in these catalytic processes,but the activity dependence on the nature of metal ions has been rarely studied due to the difficulty to compare metal complexes with different coordination *** herein reported the synthesis of a series of metal complexes of azido-substituted porphyrin(1),in which metal ions have very similar coordination *** grafting 1-M(M=Mn,Fe,Co,Ni,and Cu)onto alkynefunctionalized carbon nanotubes(CNTs)through the same covalent connection,the resulted hybrids 1-M@CNT were all active and robust for both electrocatalytic HER and OER in alkaline aqueous *** these hybrids,1-Fe@CNT displayed the highest electrocatalytic activity for HER,while 1-Co@CNT was the most active one for ***,a two-electrode water electrolysis cell assembled with 1-Fe@CNT as the cathode and 1-Co@CNT as the anode required smaller applied bias potential by210 mV to get 10 mA/cm^(2)current density as compared to that assembled with Pt/C and Ir/C with the same amount of metal *** work is significant to correlate HER and OER activity with the nature of first-row transition metal ions and to highlight promising potential applications of molecular electrocatalysis in water splitting.

关键词： Metal porphyrins Molecular electrocatalysis Hydrogen evolution Oxygen evolution Water splitting

A simple structure copolymer donor based on carboxylated benzodithiophene for polymer solar cells

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Science China Chemistry 2022年第9期65卷 1775-1781页

作者： Xiaochen Wang Rui Zhao Zicheng Ding Shengzhong(Frank)Liu Yongfang Li School of Materials Science and Engineering Shaanxi Normal UniversityXi’an 710119China shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologyShaanxi Normal UniversityXi’an 710119China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

The design and development of low-cost and efficient photovoltaic materials remain a major challenge for the research and application of polymer solar cells(PSCs).Therefore,developing efficient photovoltaic polymers with simple structure and easy preparation has become an important research *** we report a facilely synthesized electron-donating polymer X1 with a simple chemical structure,which is composed of carboxylated benzo[1,2-b:4,5-b′]dithiophene(BDT)and thiophene *** carboxylate substituents on the BDT unit endowed the polymer with appropriate solubility,low-lying highest occupied molecular orbital(HOMO)energy level,and superior *** PSCs based on X1 as the donor showed a high power conversion efficiency of 16.6%,with a remarkable short-circuit current density of 27.07 m A cm^(-2).These results demonstrated that X1 is a highly promising candidate for low-cost and efficient ***,this study revealed the potential of carboxylated BDT as an effective building block in the research and development of high-performance photovoltaic materials.

关键词： polymer donor carboxylate benzodithiophene(BDT) low-cost polymer solar cells(PSCs)

Hydrophilic MnO_(2) nanowires coating with o-fluoroaniline for electrocatalytic water oxidation

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Chinese Journal of Structural Chemistry 2023年第8期42卷 31-36页

作者： Lingshuang Qin Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education and School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an710119China

In the active Mn_(4)CaO_(5) cluster of the natural water oxidation system,one of the dangling Mn atoms is surrounded by water molecules through coordination and hydrogen *** means that the enrichment of water molecules around the Mn catalysts has a positive effect on the water oxidation *** by nature photosynthesis,the hydrophilic surfaces are believed to be able to capture water molecules to assist water ***,we report MnO_(2)@PFANI nanowires with improved mass transfer efficiency and conductivity for electrocatalytic water *** as-prepared nanowires are synthesized by coating hydrophilic polymers on MnO_(2) *** hydrophilic surface captures water molecule and promotes mass transfer processes,and the conductivity of the polymer can also increase charge transfer *** reach a current density of 10 mA cm^(-2),a low overpotential of 440 mV is required in a 1.0 M KOH solution for the MnO_(2)@PFANI *** hydrophilicity and conductivity are systematically investigated by both physical and electrochemical *** study provides a surface engineering idea for the fabrication of efficient electrocatalysts.

关键词： Electrocatalysis Oxygen evolution reaction MnO_(2) Hydrophilicity Conductivity

Predicting Microbe-Disease Association Based on Heterogeneous Network and Global Graph Feature Learning

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Chinese Journal of Electronics 2022年第2期31卷 345-353页

作者： WANG Yueyue LEI Xiujuan PAN Yi School of Computer Science Shaanxi Normal University Department of Computer Science Georgia State University Faculty of Computer Science and Control Engineering Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences

Numerous microbes inhabit human body,making a vast difference in human health. Hence, discovering associations between microbes and diseases is beneficial to disease prevention and treatment. In this study,we develop a prediction method by learning global graph feature on the heterogeneous network(called HNGFL).Firstly, a heterogeneous network is integrated by known microbe-disease associations and multiple *** on microbe Gaussian interaction profile(GIP) kernel similarity, we consider different effects of these microbes on organs in the human body to further improve microbe similarity. For disease similarity network, we combine GIP kernel similarity, disease semantic similarity and disease-symptom similarity. And then, an embedding algorithm called GraRep is used to learn global structural information for this network. According to vector feature of every node, we utilize support vector machine classifier to calculate the score for each microbe-disease pair. HNGFL achieves a reliable performance in cross validation, outperforming the compared methods. In addition, we carry out case studies of three diseases. Results show that HNGFL can be considered as a reliable method for microbe-disease association prediction.

关键词： microorganisms global graph feature learning support vector machines patient diagnosis global structural information disease semantic similarity disease-symptom similarity HNGFL pattern classification graph theory microbe Gaussian interaction profile kernel similarity bioinformatics support vector machine classifier GraRep diseases learning (artificial intelligence) microbe-disease association prediction heterogeneous network Gaussian processes GIP kernel similarity

Synthesis,Structure and Luminescence Properties of Dumbbell-like Silver Clusters

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Chinese Journal of Structural Chemistry 2020年第10期39卷 1824-1834,1743页

作者： DING Shu-Ping ZHANG Zong-Yao ZHOU Guo-Jun CAO Rui School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an 710119China Department of Chemistry Renmin University of ChinaBeijing 100872China)versity of China

In this work,three stable dumbbell-shaped silver clusters 1~3,formed by a novel bifunctional ligand Ph2P-C6H4-3-C=CH,are *** three complexes have cage structures constructed with thirty-six silver atoms,which are templated by chloride *** the self-assembly process of silver acetylides,argentophilic interactions and Ag(I)-ethynide interactions are important for the formation of silver cores to yield a diversity of silver *** molecular interactions(π-π,C-H…π,C-H…F,C-H…O)are also found in these complexes,which are crucial to stabilizing these silver *** with simple alkynyl ligands(RC≡C-),the introduction of phosphine groups into alkynyl ligand can effectively control the undesired infinite growth of silver *** photophysical behaviors of complexes 1~3 are studied,showing intense orange roomtemperature luminescence in the solid state upon the exposure to UV *** luminescence mainly arises from ligand-to-metal charge transfer(LMCT)and metal-cluster-centered transitions(MC)within the silver clusters.

关键词： silver cluster argentophilic interaction bifunctional ligand Ag(I)-ethynide interaction luminescence

Phase-transfer synthesis of α-Co(OH)_2 and its conversion to CoO for efficient electrocatalytic water oxidation

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Science Bulletin 2017年第9期62卷 626-632页

作者： Dingyi Guo Fangfang Chen Wei Zhang Rui Cao School of Chemistry and Chemical Engineering Shaanxi Normal University Department of Chemistry Renmin University of China

Water splitting is an attractive way to produce recyclable hydrogen energy resource. The oxygen evolution reaction(OER) is the rate-determine step of water electrolysis. The exploring of low-cost, highly efficient and durable electrocatalysts for OER is thus extremely important. In this work, we developed a facile two-phase protocol to fabricate an α-Co(OH)_2 using sodium oleate as the phase-transfer *** crystallinity and structure of the α-Co(OH)_2 was regulated by heat treatments toward enhanced electrocatalytic OER activity. With the calcination of the as-prepared α-Co(OH)_2 at 200 °C, a networked and well-dispersed CoO nanoparticles were formed. The CoO sample afforded an OER current density of 10 mA cm^(-2) under a low overpotential of 312 mV in a 1 mol L^(-1) KOH aqueous solution. The high activity of the CoO material is believed to be associated with its ultra-small particle size and plentiful open spaces in the material, both of which can provide abundant surface catalytic sites.

关键词： Water oxidation Cobalt oxide Cobalt hydroxide Oxygen evolution reaction Electrocatalysis