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Plasma induced grain boundaries to boost electrochemical reduction of CO2 to formate

Journal of Energy Chemistry 2024年第8期95卷 636-643页

作者： Guan Wang Shengtao Zhong Xiaoqian Xiong Jing Li Fangyuan Wang Li Huo Daoxiong Wu Xingqi Han Zhitong Wang Qi Chen Xinlong Tian Peilin Deng School of marine Science and Engineering State Key Laboratory of Marine Resource Utilization in South China Sea Hainan University

Bismuth-based catalysts are highly promising for the electrochemical carbon dioxide reduction reaction（eCO2RR） to formate product.However,achieving high activity and selectivity towards formate and ensuring long-term stability remains challenging.This work reports the oxygen plasma inducing strategy to construct the abundant grain boundaries of Bi/BiOxon ultrathin two-dimensional Bi nanosheets.The oxygen plasma-treated Bi nanosheet（OP-Bi） exhibits over 90% Faradaic efficiency（FE） for formate at a wide potential range from-0.5 to-1.1 V,and maintains a great stability catalytic performance without significant decay over 30 h in flow cell.Moreover,membrane electrode assembly（MEA） device with OPBi as catalyst sustains the robust current density of 100 mA cm-2over 50 h,maintaining a formate FE above 90%.In addition,rechargeable Zn-CO2battery presents the peak power density of1.22 mW cm-2with OP-Bi as bifunctional catalyst.The mechanism experiments demonstrate that the high-density grain boundaries of OP-Bi provide more exposed active sites,faster electron transfer capacity,and the stronger intrinsic activity of Bi atoms.In situ spectroscopy and theo retical calculations further elucidate that the unsaturated Bi coordination atoms between the grain boundaries can effectively activate CO2molecules through elongating the C-O bond,and reducing the formation energy barrier of the key intermediate（*OCOH）,thereby enhancing the catalytic performance of eCO2RR to formate product.

关键词： Bi nanosheet CO2 electroreduction Grain boundary MEA device Unsaturation Bi atoms

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Metal complexes of bipyridine-functionalized covalent organic frameworks as efficient electrocatalysts for oxygen evolution reaction

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Rare Metals 2024年第7期43卷 3096-3106页

作者： Zhuang-Zhuang Wu Tian Xia Ying Liang Yong-Peng Li Zhu-Yin Sui Li-Juan Feng Dao-Xiong Wu Xin-Long Tian Qi Chen state key laboratory of marine Resource utilization in south china sea School of Marine Science and EngineeringHainan University School of Chemistry and Chemical Engineering Yantai University School of Bioengineering Zhuhai Campus of Zunyi Medical University

Electrocatalytic water splitting is considered a clean and practic al method for producing energy.In this study,COF-Bpy,a bipyridine-functionalized covalent organic framework（COF）,was prepared via post-synthetic modification,after which electrocatalysts for the oxygen evolution reactions（OER） were formed through coordination to single- or double-transition metals（Fe,Co,Ni,FeCo,FeNi or CoNi）.COF-Bpy@FeNi delivered the best OER performance among the studied electrocatalysts,with an overpotential of 399 mV at 10 mA·cm-2in an alkaline electrolyte(1.0 mol·L-1KOH aqueous).Notably,the electrocatalytic performance of COF-Bpy@FeNi showed slight degradation during durability testing,which is ascribable to its irreversible benzoquinoline structure and strong metal coordination.As expected,COF-Bpy@FeNi exhibited a low overpotential of 347 mV at a turnover frequency（TOF） of 0.1 s-1,which suggests that COF-Bpy@FeNi possesses excellent intrinsic electroc atalytic OER activity.Finally,density functional theory（DFT） calculations reveal that the Ni site plays a major role,while the Fe site adjusts the electronic structure of the Ni ions,which rationalizes the excellent OER properties of COF-Bpy@FeNi.This study not only provides a simple and efficient method for complexing COFs with transition metals,but also offers a novel strategy for designing porous organic polymer electrocatalysts.

关键词： Covalent organic framework Oxygen evolution reactions (OER) electrocatalyst Nickel–iron synergy Water splitting

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A universal and ultrafast method for fabricating a library of nanocellulose-supported metal nanoparticles

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Progress in Natural Science:Materials International 2024年第2期34卷 389-395页

作者： Ziyi Luo Xiaoyang Wang Baihua Cui Hao Luo Tao Zhang Jia Ding Yanan Chen Yida Deng Wenbin Hu School of Materials Science and Engineering Tianjin University Department of Chemistry National University of Singapore state key laboratory of marine Resource utilization in south china sea School of Materials Science and Engineering Hainan University

Using nanocatalysts to catalyze water electrolysis for hydrogen production is an ideal solution to address the energy crisis.The most well-adopted fabrication methods for nanocatalysts are tube furnace annealing,Hydrothermal method,etc.,hardly satisfying the trade-off among coarsening,dispersity,and particle size due to mutual restrictions.Herein,a universal,ultrafast and facile cellulose nanometer whiskers-high temperature shock（CNWHTS） method was reported for fabricating a library of ultrafine metal nanoparticles with uniform dispersion and narrow size distribution.The metal-anchor functional groups in CNW（i.e.,-OH and-COOH） and the characteristics of the HTS method for ultrafast heating and powerful quenching synergistically contribute to the successful synthesis of metal nanoparticles.As an initial demonstration,the as-prepared Pt nanocatalyst(η10 mA cm-2=51.8 mV) shows more excellent catalytic hydrogen evolution reaction（HER） performance than the Pt catalyst prepared in the tubular furnace(η10 mA cm-2=169.4 mV).This rapid and universal CNW-HTS method can pave the way for nanomanufacturing to produce high-quality metal nanoparticles,thereby expanding applications of energy conversion and electrocatalysis.

关键词： Electrocatalysis High-temperature shock Hydrogen evolution reaction (HER) Nanocellulose Nanomanufacturing Nanoparticles

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Accurate identification of glass crystallization helps in selecting high electronic conductivity materials

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Progress in Natural Science:Materials International 2024年第3期34卷 503-511页

作者： Fanhou Kong Shuli Li Suoqi Zhao Huiwen Li Lin Li Zhenting Zang Rui Zhang Hongrui Liu Lehan Wang Changjiu Li Keng H.Chung Dongying key laboratory of New Energy Materials and Devices & School of Chemical Engineering Shandong Institute of Petroleum and Chemical Technology Special Glass key Lab of Hainan Province & state key laboratory of marine Resource utilization in south china sea Hainan University

Though the current research on vanadium-based glass electrodes has made great progress, the conductivity theory of V-based glasses has not been obviously improved and crystals cannot be positioned precisely. The changes in the valence state of V3+, V4+and V5+are regulated by the strong reducing agent Fe2P to realize valence bond transformation of the amorphous electrode, explore the redox process of multi-electron reactions and further optimize the conductivity of electrode materials. VPFe2 and VPFe3 precipitate VO2crystals and VPFe4 precipitates VO2and V6O11crystals. Electron back-scattered diffraction was used to accurately identify the distribution and specific positions of both types of crystals. V6O11crystals exhibit a strong texture according to pole figure and inverse pole figure. XPS reveals that Fe2P and V2O5, undergo a redox reaction during the hightemperature melting process, where V5+is reduced to V4+and V3+and V4+renders a positive influence on conductivity. The addition of Fe2P increases the content of V4+in the glass and VPFe3 glass contains the highest content of V4+, leading to the highest electronic conductivity. V2O5transforms into VO2crystals and VO2transforms into V6O11with the increase of Fe2P content. The type of nanocrystal precipitation in glass affects electronic conductivity.

关键词： Electron back-scattered diffraction Electronic conductivity Glass crystallization Multi-electron reactions V2O5

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Spontaneous anchoring Cl into α-Co（OH）2 as efficient and stable oxygen reduction electrocatalysts for seawater battery

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Rare Metals 2024年第7期43卷 3074-3083页

作者： Wang Zheng Xue-Rong Zheng Qi Lu Yan-Hui Cao Yang Wang Hai-Peng Fu Jin-Feng Zhang Yi-Da Deng Wen-Bin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin University state key laboratory of marine Resource utilization in south china sea School of Materials Science and EngineeringHainan University key laboratory of Electromagnetic Processing of Materials Ministry of EducationNortheastern University

seawater battery is an advanced energy storage system that enables conversion of chemical energy to electricity by consuming metals,dissolved oxygen and seawater in anode,cathode and electrolyte,respectively.However,the oxygen reduction reaction（ORR） activity and stability of electrocatalysts can be easily deactivated due to the severe Cl-permeation and corrosion in seawater electrolyte.Herein,we developed a structural buffer engineering strategy by spontaneously anchoring Cl-into α-Co（OH）2as efficient and stable ORR electrocatalysts,in which the ultrathin α-Co（OH）2nanosheets were synthesized using an ultrafast solution high-temperature shock（SHTS） strategy.The large lattice space（～ 0.8 nm） of layered α-Co（OH）2ensured the spontaneously penetration of Cl-into the lattice structure and replaced part of OH-to form α-Co（OH）2-xClx.The continuous leaching and compensating of saturated Cl in α-Co（OH）2-xClxcould enhance the Cl-corrosion resistance and modulate electronic structure of Co metallic sites,thus improving the ORR electrocatalytic activity and stability in seawater electrolyte.The α-Co（OH）2-xClxseawater batteries display superior onset and half-wave potentials of 0.71 and 0.66 V,respectively,which are much better than the counterparts of α-Co（OH）2and of β-Co（OH）2with no Cl-penetrating and no buffer structure.The α-Co（OH）2-xClx-based seawater batteries display stable open-circuit potential of 1.69 V and outstanding specific capacity of 1345 mAh·g-1.

关键词： seawater battery Oxygen reduction electrocatalyst Solution high-temperature shock Structural buffer engineering

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Polyp-Canal Reconstruction Reveals Evolution Toward Complexity in Corals

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Research 2024年第1期2023卷 417-428页

作者： Yixin Li Xin Liao Xin Wang Yuanchao Li Hongwei Zhao Yunpeng Zhao Junyuan Chen Chunpeng He Zuhong Lu state key laboratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China state key laboratory of Coastal and Offshore Engineering Dalian University of TechnologyDalian 116024China Guangxi key Lab of Mangrove Conservation and utilization Guangxi Mangrove Research CenterGuangxi Academy of SciencesBeihai 536000China Hainan Academy of Ocean and Fishery Sciences Haikou 571126China state key laboratory of marine resources utilization in south china sea Hainan UniversityHaikou 570228China Nanjing Institute of Geology and Palaeontology Chinese Academy of Sciences39 East Beijing RoadNanjing 210008China

Modern scleractinian corals are classified into robust,complex,and basal clades through comparative molecular studies.However,only few morphological or biological criteria can systematically determine the evolutionary trajectories of these major scleractinian coral clades.Here,we obtained the structural information of 21 scleractinian coral species representing robust and complex clades:High-resolution micro-computed tomography was used to reconstruct the polyp-canal systems in their colonies and to visualize the dynamic polyp growth processes.We found that the emergence of mesh-like canals may distinguish representatives of complex and robust clades.The differences in polyp-canal connections suggest distinct evolutionary trajectories among coral species:The formation of the canal network promoted the development of more complex coral structures,and coral polyps within this network formed calices of very similar volume,following precise axial growth directions.The influence of individual polyps on the coral colony becomes less significant as coral structures become more complex,and coral species with more complicated polyp-canal systems occupied niches more efficiently.This work supplements current evolutionary studies on reef-building corals,providing insight for further studies on coral growth patterns.

关键词： Coral representing directions

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Small molecule deoxynyboquinone triggers alkylation and ubiquitination of Keap1 at Cys489 on Kelch domain for Nrf2 activation and inflammatory therapy

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Journal of Pharmaceutical Analysis 2024年第3期14卷 401-415页

作者： Ke-Gang Linghu Tian Zhang Guang-Tao Zhang Peng Lv Wen-Jun Zhang Guan-Ding Zhao Shi-Hang Xiong Qiu-Shuo Ma Ming-Ming Zhao Meiwan Chen Yuan-Jia Hu Chang-Sheng Zhang Hua Yu state key laboratory of Quality Research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao SARChina Macao Centre for Research and Development in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao SARChina key laboratory of Tropical marine Bio-resources and Ecology Guangdong Key Laboratory of Marine Materia MedicaRNAM Center for Marine MicrobiologySouth China Sea Institute of OceanologyChinese Academy of SciencesGuangzhou510301China state key laboratory of Functions and Applications of Medicinal Plants&School of Pharmaceutical Sciences Guizhou Medical UniversityGuiyang550025China

Activation of nuclear factor erythroid 2-related factor 2(Nrf2)by Kelch-like ECH-associated protein 1(Keap1)alkylation plays a central role in anti-inflammatory therapy.However,activators of Nrf2 through alkylation of Keap1-Kelch domain have not been identified.Deoxynyboquinone(DNQ)is a natural small molecule discovered from marine actinomycetes.The current study was designed to investigate the anti-inflammatory effects and molecular mechanisms of DNQ via alkylation of Keap1.DNQ exhibited significant anti-inflammatory properties both in vitro and in vivo.The pharmacophore responsible for the anti-inflammatory properties of DNQ was determined to be theα,β-unsaturated amides moieties by a chemical reaction between DNQ and N-acetylcysteine.DNQ exerted anti-inflammatory effects through activation of Nrf2/ARE pathway.Keap1 was demonstrated to be the direct target of DNQ and bound with DNQ through conjugate addition reaction involving alkylation.The specific alkylation site of DNQ on Keap1 for Nrf2 activation was elucidated with a synthesized probe in conjunction with liquid chromatography-tandem mass spectrometry.DNQ triggered the ubiquitination and subsequent degradation of Keap1 by alkylation of the cysteine residue 489(Cys489)on Keap1-Kelch domain,ultimately enabling the activation of Nrf2.Our findings revealed that DNQ exhibited potent anti-inflammatory capacity throughα,β-unsaturated amides moieties active group which specifically activated Nrf2 signal pathway via alkylation/ubiquitination of Keap1-Kelch domain,suggesting the potential values of targeting Cys489 on Keap1-Kelch domain by DNQ-like small molecules in inflammatory therapies.

关键词： Deoxynyboquinone Anti-inflammation Target Keap1/Nrf2 Alkylation Ubiquitination

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Graphdiyne oxide substrate-enhanced peroxidase-mimicking performance of Ru nanoparticles with physiological pH preference

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Nano Research 2024年第3期17卷 1123-1131页

作者： Cong Xu Wenjie Ma Haozhi Wang Leihou Shao Weiqi Li Ping Yu Lanqun Mao Beijing National laboratory for Molecular Science Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China state key laboratory of marine Resource utilization in south china sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China College of Chemistry Beijing Normal UniversityBeijing 100875China

Modulating electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in the field of catalytic science.However,the roles of supporting substrates in regulating catalytic properties of nanozymes remain elusive.In this study,we find that the use of graphdiyne oxide(GDYO)as the substrate for self-terminating growth of Ru nanoparticles(Ru@GDYO)endows the peroxidase-like activity of Ru nanoparticles with intrinsic physiological pH preference and natural horseradish peroxidase(HRP)comparable performance.Ru nanoparticles electrolessly deposited onto GDYO possess a partially oxidized electronic structure owing to limited charge transfer between Ru and GDYO,contributing to the intrinsic physiological pH preference of the peroxidase-mimicking nanozyme.More importantly,the substrate GDYO plays an influential factor in enhancing catalytic activity,that is,the activity of Ru@GDYO is much higher than that of Ru nanoparticles deposited on other carbon substrates including graphene oxides and graphdiyne.To demonstrate the application of Ru@GDYO nanozyme in neutral solutions,we employ Ru@GDYO with nicotinamide adenine dinucleotide(NAD+)-dependent dehydrogenases in physiological conditions to realize a sustainable cascade reaction by means of forming continuous NAD^(+)/dihydronicotiamide adenine dinucleotide(NADH)recycling.Our finding represents a promising perspective on designing high-performance peroxidase-mimicking nanozymes with broader applicability,raising fundamental understanding of structure–activity relationship,and investigating new applications of nanozymes in biological systems.

关键词： nanozyme graphdiyne reactive oxygen species electroless deposition metal–support interaction

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Diagnostic Study of an Extreme Explosive Cyclone over the Kuroshio/Kuroshio Extension Region

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Journal of Ocean University of china 2024年第3期23卷 605-617页

作者： ZHANG Shuqin LIAO Qinghua LIU Chunlei GAO Xiaoyu LONG Jingchao LI Pengyuan XU Jianjun College of Ocean and Meteorology Guangdong Ocean UniversityZhanjiang 524088China south china sea Institute of marine Meteorology Guangdong Ocean UniversityZhanjiang 524088China CMA-GDOU Joint laboratory for marine Meteorology Guangdong Ocean UniversityZhanjiang 524088China key laboratory of Climate Resources and Environment in Continental Shelf Sea and Deep Sea of Department of Education of Guangdong ProvinceGuangdong Ocean UniversityZhanjiang 524088China state key laboratory of Severe Weather Chinese Academy of Meteorological SciencesBeijing 100081China Department of marine Meteorology Ocean-Atmosphere Interaction and Climate LaboratoryKey Laboratory of Physical OceanographyOcean University of ChinaQingdao 266100China

Explosive cyclones(ECs)occur frequently over the Kuroshio/Kuroshio Extension region.The most rapidly intensified EC over the Kuroshio/Kuroshio Extension region during the 42 years(1979-2020)of cold seasons(October-April)was studied to reveal the variations of the key factors at different explosive-developing stages.This EC had weak low-level baroclinicity,mid-level cyclonic-vorticity advection,and strong low-level water vapor convergence at the initial explosive-developing stage.The low-level baroclinicity and mid-level cyclonic-vorticity advection increased substantially during the maximum-deepening-rate stage.The diagnostic analyses using the Zwack-Okossi equation showed that diabatic heating was the main contributor to the initial rapid intensification of this EC.The cyclonic-vorticity advection and warm-air advection enhanced rapidly in the middle and upper troposphere and contributed to the maximum rapid intensification,whereas the diabatic heating weakened slightly in the mid-low troposphere.The relative contribution of the diabatic heating decreased from the initial explosive-developing stage to the maximum-deepening-rate stage due to the enhancement of other factors(the cyclonic-vorticity advection and warm-air advection).Furthermore,the physical factors contributing to this EC varied with the explosive-developing stage.The non-key factors at the initial explosive-developing stage need attention to forecast the rapid intensification.

关键词： explosive cyclone diabatic heating cyclonic-vorticity advection rapid intensification the Kuroshio/Kuroshio Extension region

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Phase transfer-based high-efficiency recycling of precious metal electrocatalysts

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Green Chemical Engineering 2024年第1期5卷 68-74页

作者： Qing Zeng Shaonan Tian Yu Zhang Hui Liu Dong Chen Xinlong Tian Chaoquan Hu Jun Yang state key laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China state key laboratory of marine Resource utilization in south china sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou570228China Nanjing IPE Institute of Green Manufacturing Industry Nanjing211100China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Recycling precious metals with high-efficiency is undoubtedly beneficial to optimize resource utilization for environmental remediation and sustainable development.Herein,we report an efficient route to recycle the palladium(Pd)and platinum(Pt)electrocatalysts using a phase transfer method.This strategy involves acidic dissolution of deactivated precious metal(Pd/Pt)electrocatalysts from their loading substrates,mixing with an ethanolic solution of dodecylamine(DDA),subsequent extraction of metal ions into a non-polar organic phase,and final reduction by sodium borohydride to reproduce high-performance electrocatalysts towards typical electrochemical reactions,e.g.,oxygen reduction reaction(ORR)and ethanol oxidation reaction(EOR).In specific,the transfer efficiencies are up to 98%and the final recovery rate is over 85%for Pd and Pt electrocatalysts in each cycle.This approach symbolizes a facile and efficient way to recover precious metals,which might be applied to recycling a wide range of metals in various realms after appropriate modifications.

关键词： Precious metal Phase transfer Extraction Recovery Electrocatalyst

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