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Journal of Environmental Sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong anhui engineering research center of carbon neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China School of Chemistry and Chemical engineering Anqing Normal UniversityAnqing 246011China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and ***,their low durability and recyclability limit practical *** this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous *** characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular ***,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly *** work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts.

关键词： durability selectivity catalyst

Recent advances and applications of single atom catalysts based electrochemical sensors

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Nano research 2024年第4期17卷 2994-3013页

作者： Mingyue Wang Mingfu Ye Jieyue Wang Yong Xu Zhendong Wang Xinyue Tong Xinya Han Kui Zhang Wenhai Wang Konglin Wu Xianwen Wei Institute of Clean Energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China School of Materials Science and engineering Anhui University of TechnologyMaanshan 243002China anhui International research center of Energy materials green manufacturing and biotechnology School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China carbon Cycle and Emission Control research center Low-Carbon Research InstituteAnhui University of TechnologyMaanshan 243002China

Single atom catalysts(SACs)have attracted considerable attention due to their unique structures and excellent catalytic performance,especially in the area of catalysis science and energy conversion and *** recent years,SACs have emerged as a new type of sensing material for constructing electrochemical sensors(ECSs),presenting excellent sensitivity,selectivity,and ***,we review the recent advances of SACs in electrochemical sensing and discuss the status quo of current SAC-based ***,the fundamentals of SAC-based ECSs are outlined,including the involved central metal atoms and various supports of SACs in this field,the detection mechanisms,and improving strategies of SAC-based ***,the important applications of SAC-based ECSs are listed and classified,covering the detection of reactive oxygen and nitrogen species,environmental pollutants,disease biomarkers,and ***,based on abundant reported cases,the current conundrums of SAC-based ECSs are summarized,and the prediction of their future developing trends is also put forward.

关键词： single atom catalysts(SACs) electrochemical sensors(ECSs) reactive oxygen and nitrogen species environmental pollutants disease biomarkers pharmaceuticals

Effect of carbon material and surfactant on ink property and resulting surface cracks of fuel-cell microporous layers

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Chinese Journal of Chemical engineering 2024年第5期69卷 1-12页

作者： Zhekun Chen Weitong Pan Longfei Tang Xueli Chen Fuchen Wang engineering research center of Resource Utilization of carbon-containing Waste with carbon neutrality Ministry of EducationEast China University of Science and TechnologyShanghai 200237China Key Laboratory of Pressure Systems and Safety Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

Ensuring the consistency of electrode structure in proton-exchange-membrane fuel cells is highly desired yet challenging because of wide-existing and unguided cracks in the microporous layer(MPL). The first thing is to evaluate the homogeneity of MPL with cracks quantitatively. This paper proposes the homogeneity index of a full-scale MPL with an area of 50 cm~2, which is yet to be reported in the literature to our knowledge. Besides, the effects of the carbon material and surfactant on the ink and resulting MPL structure have been studied. The ink with a high network development degree produces an MPL with low crack density, but the ink with high PDI produces an MPL with low crack homogeneity. The polarity of the surfactant and the non-polarity of polytetrafluoroethylene(PTFE) are not mutually soluble,resulting in the heterogeneous PTFE distribution. The findings of this study provide guidelines for MPL fabrication.

关键词： Proton-exchange-membrane fuel cell Microporous layer Crack density Crack homogeneity Polytetrafluoroethylene distribution Surfactant

In situ meso-tetra(4-carboxyphenyl)porphyrin ligand substitution in Hf-MOF for enhanced catalytic activity and stability in photoredox reactions

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Rare Metals 2024年第6期43卷 2682-2694页

作者： Jie Hu Hong-Xin Lao Xiu-Wu Xu Wei-Kang Wang Le-Le Wang Qin-Qin Liu School of Materials Science and engineering Jiangsu UniversityZhenjiang 212013China College of Chemistry and Materials Engineering Research Center of Carbon NeutralityAnhui Normal UniversityWuhu 241002China Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contaminants Putian UniversityPutian 351100China

Though there are numerous intrinsic merits of metal-organic frameworks(MOFs),low charge separation efficiency has imposed heavy restrictions on their photocatalytic ***,in situ porphyrin ligand substitution,as a strategy for improving the charge separation efficiency and increasing the amounts of active sites,has been designed and realized in a Hf-biphenyl dicarboxylic acid(BPDC)***,a size and geometry matched meso-tetra(4-carboxyphenyl)porphyrin(TCPP)ligand was selected and doped into Hf-BPDC MOF by forming coordinating bonds with Hf centers,forming dualligand Hf-BPDC-TCPP *** resultant Hf-BPDC-TCPP MOF showed significantly improved activity and chemical stability in the photocatalytic H_(2)generation(261μmol·g^(-1)·h^(-1))and tetracycline(TC)degradation reactions(95.8%),which was 48 and 1.47 folds higher than that of the Hf-BPDC *** and electrochemical studies revealed that the introduction of porphyrin ligand could generate a stronger internal electric field for boosting the charge separation and transfer,increase the specific surface area for providing more active sites,and narrow the band gap to enhance the visible light *** in situ ligand substitution method provides a promising approach to build a tunable platform for constructing high-performance MOF photocatalysts.

关键词： Ligand substitution Metal organic frameworks Meso-tetra(4-carboxyphenyl)porphyrin Hydrogen evolution reaction Tetracycline degradation

Jellyfish bio-inspired Fe@CNT@CuNC derived from ZIF-8 for cathodic oxygen reduction

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Nano research 2024年第4期17卷 2352-2359页

作者： Kai Cheng Zequan Liu Demin Jiang Min Song Yuqiao Wang research center for Nano Photoelectrochemistry and Devices School of Chemistry and Chemical EngineeringSoutheast UniversityNanjing 211189China Yangtze River Delta carbon neutrality Strategy Development Institute Southeast UniversityNanjing 210096China School of Energy and Environment Southeast UniversityNanjing 210096China

Biomimetics provides guidance to design and synthesize advanced catalysts for oxygen reduction reaction in microbial fuel cells(MFCs).Herein,jellyfish-inspired Fe clusters on carbon nanotubes connected with CuNC(Fe@CNT@CuNC)were designed and prepared by using zeolitic imidazolate framework(ZIF)-8 precursors to imitate the organic texture and function of *** antibacterial effect of Cu^(+)ions depressed the growth of cathode biofilm to ensure rapid mass *** clusters and CuNC connected by CNTs accelerated the electron transfer from Fe to *** optimization of oxygen adsorption was caused by electron redistribution between sites of Fe and ***-like catalysts achieved a half-wave potential of 0.86 V and onset potential of 0.95 V *** hydrogen electrode(RHE).MFCs gained the maximum power density of 1600 mW·m^(-2) after 500 h *** work provides insights into the special design of advanced catalysts based on bio-inspiration and biomimetics.

关键词： bio-inspiration oxygen reduction reaction antibacterial ability microbial fuel cells density functional theory(DFT)rational design

On-demand engineerable visible spectrum by fine control of electrochemical reactions

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National Science Review 2024年第3期11卷 239-249页

作者： Qirong Liu Lei Liu Yongping Zheng Min Li Baofu Ding Xungang Diao Hui-Ming Cheng Yongbing Tang Advanced Energy Storage Technology research center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences Institute of Technology for carbon neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences School of Energy and Power engineering North University of China School of Resource Environment and Safety EngineeringHunan University of Science and Technology School of Energy and Power engineering Beihang University Shenzhen Key Laboratory of Energy Materials for carbon neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences

Tunability of optical performance is one of the key technologies for adaptive optoelectronic applications,such as camouflage clothing, displays, and infrared shielding. High-precision spectral tunability is of great importance for some special applications with on-demand adaptability but remains challenging. Here we demonstrate a galvanostatic control strategy to achieve this goal, relying on the finding of the quantitative correlation between optical properties and electrochemical reactions within materials. An electrochromic electro-optical efficiency index is established to optically fingerprint and precisely identify electrochemical redox reactions in the electrochromic device. Consequently, the charge-transfer process during galvanostatic electrochemical reaction can be quantitatively regulated, permitting precise control over the final optical performance and on-demand adaptability of electrochromic devices as evidenced by an ultralow deviation of research in a wide range of spectroelectrochemistry, electrochemical energy storage, electrocatalysis, and material chemistry.

关键词： electrochromics fine control spectral tunability high precision galvanostatic control

Phase field modeling of grain stability of nanocrystalline alloys by explicitly incorporating mismatch strain

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Rare Metals 2024年第7期43卷 3370-3382页

作者： Min Zhou Hong-Hui Wu Yuan Wu Hui Wang Xiong-Jun Liu Sui-He Jiang Xiao-Bin Zhang Zhao-Ping Lu Beijing Advanced Innovation center for Materials Genome engineering State Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology Beijing Institute for carbon neutrality University of Science and Technology Institute of Materials Intelligent Technology Liaoning Academy of Materials

Ab st ra ct Nanocrystalline materials exhibit unique properties due to their extremely high grain boundary(GB) ***,this high-density characteristic induces grain coarsening at elevated temperatures,thereby limiting the widespread application of nanocrystalline *** experimental observations revealed that GB segregation and second-phase pinning effectively hinder GB migration,thereby improving the stability of nanocry stalline *** this study,a mouified phase-field model that integrates mismatch strain,solute segregation and precipitation was developed to evaluate the influence of lattice misfit on the thermal stability of nanocrystalline *** simulation results indicated that introducing a suitable mismatch strain can effectively enhance the microstructural stability of nanocrystalline *** synergizing precipitation with an appropriate lattice misfit,the formation of second-phase particles in the bulk grains can be suppressed,thereby facilitating solute segregation/precipitation at the *** concentrated solute segregation and precipitation at the GBs effectively hinders grain migration,thereby preventing grain *** findings provide a new perspective on the design and regulation of nanocrystalline alloys with enhanced thermal stability.

关键词： Phase field model Mismatch strain Second-phase precipitation Grain boundary segregation Nanocrystalline alloys

Tuning the local coordination environment of silver(Ⅰ) coordination networks with counterions for enhanced electrocatalytic CO_(2) reduction

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Science China Chemistry 2024年第5期67卷 1524-1530页

作者： Xiaofeng Cui Xueting Wang Cong Fu Bing Liu Mei-Yan Gao Tingting Kong Yujie Xiong anhui engineering research center of carbon neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Department of Chemical Sciences Bernal InstituteUniversity of LimerickLimerick V94 T9PXRepublic of Ireland School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China School of Chemical and Material engineering Jiangnan UniversityWuxi 214122China

Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and intermediate stabilization. It is imperative to elucidate the mechanism for such an influence towards the rational design of efficient catalysts;however, the complex interactions between the multiple factors involved in the system make it challenging to establish a clear structure–performance relationship. In this work, we chose ion-intercalated silver(I)-based coordination networks(AgCNs) with a well-defined structure as a model platform, which enables us to understand the regulation mechanism of counterions as the counterions are the only tuning factor involved in such a system. We prepared two isostructural Ag CNs with different intercalation ions or counterions of BF_(4)^(-) and ClO_(4)^(-)(named as AgCNs-BF_(4) and AgCNs-ClO_(4)) and found that the former has a more competitive CO_(2) electroreduction performance than the latter. AgCNs-BF_(4) achieves the highest Faradaic efficiency for CO_(2) to CO of 87.1% at-1.0 V(vs. RHE) with a higher partial current density, while AgCNs-ClO_(4) exhibits only 77.2% at the same applied *** characterizations and theoretical calculation reveal that the presence of BF_(4)^(-)is more favorable for stabilizing the COOH^(*) intermediate by weakening hydrogen bonds, which accounts for the superior activity of Ag CNs-BF_(4).

关键词： electrocatalytic CO_(2) reduction coordination networks local environment counterions intercalation ions

Efficient piezo-catalytic dye degradation using piezoelectric 6H-SiC under harsh conditions

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Rare Metals 2024年第7期43卷 3173-3184页

作者： Lin-Lin Zhou Tao Yang Kang Wang Lai-Pan Zhu En-Hui Wang Kuo-Chih Chou Hai-Long Wang Xin-Mei Hou Institute for carbon neutrality University of Science and Technology Beijing Institute of Steel Sustainable Technology Liaoning Academy of Materials Beijing Institute of Nanoenergy and Nanosystems Chinese Academy of Sciences School of Materials Science engineering Zhengzhou University Beijing Advanced Innovation center for Materials Genome engineering Beijing University of Science and Technology

The development of novel piezoelectric catalysts against harsh conditions is indeed crucial for improving the piezo-catalytic degradation efficiency of colored organic dyes in *** this work,6H-SiC nanoparticles（NPs） are utilized to piezo-catalytic degrade rhodamine B（RhB） and methylene blue（MB） under ultrasonic vibration for the first *** degradation efficiency of RhB and MB reaches 98.8% and 98.7%within 80 *** piezoelectricity of 6H-SiC is comprehensively analyzed by the piezoresponse force microscope（PFM） and finite element method（FEM）.The strong oxidizing active free radicals generated by the continuous piezoelectric polarized electric field of 6H-SiC,i.e.,·O2-and·OH,induce the decomposition reactions of colored organic dyes in *** the dyes are proven to degrade to harmless or less-harmful products gradually during the piezo-catalysis process by high-performance liquid chromatography tandem mass spectrometry（HPLC-MS）.Moreover,RhB is also decomposed efficiently by 6HSiC NPs under acidic and alkaline *** results prove the feasibility of 6H-SiC for decomposing common water pollutants under harsh conditions and provide a new perspective for water purification.

关键词： Piezo-catalytic degradation 6H-SiC Rhodamine B (RhB) Methylene blue (MB) Harsh conditions

Improvement in hydrogen storage performance of MgH_(2) by vanadium doped with ZIF-8 derived a single-atom catalyst V-N-C

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Rare Metals 2024年第6期43卷 2623-2635页

作者： Fei-Fan Hong Wei-Tao Shi Ruo-Lin Zhao Yi Fan Zi-Qi Liu Si-Zhi Ding Hai-Zhen Liu Wen-Zheng Zhou Jin Guo Zhi-Qiang Lan Guangxi Novel Battery Materials research center of engineering Technology and center on Nanoenergy research Guangxi Colleges and Universities Key Laboratory of Blue Energy and Systems IntegrationCarbon Peak and Neutrality Science and Technology Development InstituteSchool of Physical Science and TechnologyGuangxi UniversityNanning 530004China Nanning engineering Technology research center for Power Transmission System of New Energy Vehicle Transportation CollegeNanning UniversityNanning 530200China

Herein,the successful preparation of a singleatom catalyst V-N-C using vanadium-doped zeolitic imidazolate framework(ZIF)-8 as a precursor is *** experimental results showed that the V-N-C had a good promoting effect on the hydrogen storage performance of MgH_(2),and the optimal addition amount of V-N-C was 10wt%.The hydrogenation and dehydrogenation apparent activation energies of 10 wt%V-N-C-catalyzed MgH_(2)were reduced by 44.9 and 53.5 kJ·mol^(-1),respectively,compared to those of additive-free MgH_(2).The 10 wt%V-N-C-catalyzed MgH_(2)could reabsorb 5.92 wt%of hydrogen in 50 min at 150℃,with a capacity retention rate of 99.1%after 30 cycles of hydrogen absorption and *** analysis showed that V-N-C was partially transformed into VN and metallic V when it was milled with MgH_(2);the in-situ-formed VN and metallic V played an important role in improving the hydrogen storage performance of MgH_(2).This approach provides a potential solution for obtaining high-performance Mg-based hydrogen storage materials through synergistic interactions between V,N and C.

关键词： MgH_(2) Hydrogen storage materials Catalyst Hydrogen storage perormance