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Apically guiding electron/mass transfer reaction induced by Ag/FeNx Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 106-116页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu Guangdong provincial laboratory of Chemistry and Fine chemical engineering Jieyang Center(Rongjiang laboratory) Guangdong University of Technology Guangzhou Key laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Key laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical Engineering Hainan Normal University School of materials and Energy Guangdong University of Technology Department of materials Science and engineering Southern University of Science and Technology

The disparity in the transfer of carriers（electrons/mass） during the reaction in zinc-air batteries（ZABs）results in sluggish kinetics of the oxygen reduction reaction（ORR） and oxygen evolution reaction（OER）,along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst（Ag-FeNx-N-C） was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional（3D） hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride（FeNx） nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeNx,of which electron accumulation in the FeNxphase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm-2.A rechargeable ZAB with Ag-FeNx-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles（500 h）,with a power density of 180 mW cm-2.Moreover,when employing AgFeNx-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm-2.Ag-FeNx-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.

关键词： Apically guiding effect Bifunctional catalysis Hollow star structure Mott-Schottky effect Zinc-air batteries

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In-situ embedded ultrafine Bi_(12)O_(17)Br_(2)nanotubes in MOF-derived hierarchical porous carbon for enhanced photocatalytic CO_(2)conversion to CO

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Journal of materials Science & Technology 2024年第4期171卷 47-53页

作者： Xing Sun Mengxia Ji Yi Zhang Qingzeng Xing Zihan Liu Nianhua Liu Emmanuel Nkudede Huaming Li Sheng Yin Jiexiang Xia School of Chemistry and chemical engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Key laboratory of Comprehensive and Highly Efficient Utilization of salt Lake Resources Qinghai Provincial Key Laboratory of Resources Chemistry of Salt LakesQinghai Institute of Salt LakesChinese Academy of SciencesXining 81008China

Increasing the utilization efficiency of photogenerated electrons is highly recognized as one of the ef-ficient approaches to boost the photocatalytic CO_(2)conversion efficiency.Herein,ZIF-67-derived porous carbon(PC)material was employed for the construction of PC@ultrafine Bi_(12)O_(17)Br_(2)nanotubes(PC@BOB NTs)composites through a facile solvothermal synthesis in order to optimize the use of excited elec-trons in the BOB NTs.Photoelectrochemical characterization results revealed that the introduction of PC material achieved a faster charge separation rate in the PC@BOB composites,ensuring more photogener-ated electrons participate in the CO_(2)adsorption and activation process.Moreover,the pore structures of ZIF-67-derived PC material provided abundant confined spaces for the enrichment of CO_(2)molecules.Af-ter 5 h of Xenon lamp irradiation,PC@BOB composites exhibited obviously increased photocatalytic CO_(2)reduction activity in the pure water.When the addition amount of PC was 5 wt%,the PC@BOB-2 com-posite showed the highest CO evolution rate of 359.70μmol/g,which was 2.95 times higher than that of the pure BOB NTs.This work provides some independent insights into the applications of Metal-Organic Framework(MOF)-derived hierarchical porous structures to strengthen the CO_(2)enrichment,as well as the excited charge utilization efficiency,thus achieving a high solar-to-fuel conversion efficiency.

关键词： Bi_(12)O_(17)Br_(2)nanotubes Hierarchical porous structure CO_(2)enrichment Charge separation CO_(2)photoreduction

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Ultra-high-rate Bi anode encapsulated in 3D lignin-derived carbon framework for sodium-ion hybrid capacitors

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Rare Metals 2024年第3期43卷 1037-1047页

作者： Ze-Hua Lin Xue-Qing Qiu Xi-Hong Zu Xiao-Shan Zhang Lei Zhong Shi-Rong Sun Shu-Hua Hao Ying-Juan Sun Wen-Li Zhang School of chemical engineering and Light industry Guangdong University of Technology(GDUT)Guangzhou510006China Jieyang Branch of Chemistry and chemical engineering Guangdong laboratory(Rongjiang laboratory) Jieyang515200China School of advanced Manufacturing Institute of Green Chemistry and Advanced MaterialsGuangdong University of TechnologyJieyang515200China

Bismuth(Bi),as an alloy-based anode material,has attracted much atte ntion in the developme nt of sodiumion hybrid capacitors(SIHCs)due to its high theoretical capacity.However,the volume expansion of the Bi-based anode during the sodiation/desodiation process results in limited rate capability.In the present work,a porous Bi-based composite was constructed by a one-step hydrothermal method,and Bi was encapsulated in ligninderived nitrogen-doped porous carbon(Bi@LNPC)after carbonization.The obtained Bi nanoparticles could effectively adapt to the strain and shorten the diffusion distance of Na^(+).In addition,porous carbon skeleton provides a rigid conductive network for electronic transportation.Therefore,the assembled sodium-ion half-cell with Bi@LNPC anode shows ultra-high-rate capability.When the current density was enhanced from 0.1 to 50 A·g^(-1),the specific capacity decreased slightly from 351.5 to 342.8 mAh·g^(-1).Even at an extremely high current density of 200 A·g^(-1),it retains 81.3%capacity retention when compared to a current density of 1 A·g^(-1).The SIHCs assembled by Bi@LNPC show a high energy density of 63 Wh·kg^(-1).This work provides an effective method for developing high-rate Bi anode materials for sodium-ion hybrid capacitors(SIHCs)and sodium-ion batteries(SIBs).

关键词： Bismuth Lignin Sodium-ion batteries Sodium-ion hybrid capacitors Rate Porous carbon

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High-yield production of porous carbon spheres derived from enzymatic hydrolysis lignin for zinc ion hybrid capacitors

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Frontiers of chemical Science and engineering 2024年第2期18卷 127-136页

作者： Tao Huang Xihong Zu Jianhui Ma Wenbin Jian Xueqing Qiu Wenli Zhang Guangdong provincial Key laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China School of advanced Manufacturing Guangdong University of TechnologyJieyang 522000China Jieyang Branch of Chemistry and chemical engineering Guangdong laboratory(Rongjiang laboratory) Jieyang 515200China

The widespread implementation of supercapacitors is hindered by the limited energy density and the pricey porous carbon electrode materials.The cost of porous carbon is a significant factor in the overall cost of supercapacitors,therefore a high carbon yield could effectively mitigate the production cost of porous carbon.This study proposes a method to produce porous carbon spheres through a spray drying technique combined with a carbonization process,utilizing renewable enzymatic hydrolysis lignin as the carbon source and KOH as the activation agent.The purpose of this study is to examine the relationship between the quantity of activation agent and the development of morphology,pore structure,and specific surface area of the obtained porous carbon materials.We demonstrate that this approach significantly enhances the carbon yield of porous carbon,achieving a yield of 22%in contrast to the conventional carbonization-activation method(9%).The samples acquired through this method were found to contain a substantial amount of mesopores,with an average pore size of 1.59 to 1.85 nm and a mesopore ratio of 25.6%.Additionally,these samples showed high specific surface areas,ranging from 1051 to 1831 m2·g^(−1).Zinc ion hybrid capacitors with lignin-derived porous carbon cathode exhibited a high capacitance of 279 F·g^(−1) at 0.1 A·g^(−1) and an energy density of 99.1 Wh·kg^(−1) when the power density was 80 kW·kg^(−1).This research presents a novel approach for producing porous carbons with high yield through the utilization of a spray drying approach.

关键词： enzymatic hydrolysis lignin porous carbon spheres spray drying zinc ion hybrid capacitors

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Production of linear alkylbenzene over Ce containing Beta zeolites

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Chinese Journal of chemical engineering 2024年第3期67卷 220-227页

作者： Shiqi Zhang Shengzhi Gan Baoyu Liu Jinxiang Dong School of chemical engineering and Light industry Guangdong Provincial Key Laboratory of Plant Resources BiorefineryGuangzhou Key Laboratory of Clean Transportation Energy ChemistryGuangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and chemical engineering Guangdong laboratory(Rongjiang laboratory) Jieyang 515200China

Ce-encapsulated Beta zeolite was synthesized by a one-pot hydrothermal method with citric acid complexing Ce in the absence of Na species.Additional citric acid can effectively prevent the deposition of Ce species during the hydrothermal synthesis of zeolites,leading to uniform distribution of Ce cluster in the framework of Beta zeolites.Moreover,the sodium-free synthesis system resulted that the Brønsted acid sites were mainly located on the straight channels and external surface of Beta zeolites,improving the utilization of Brønsted acid sites.In addition,Ce encapsulated Beta zeolites showed enhanced activity and robust stability in the alkylation of benzene with 1-dodecene based on the synergistic effect between Ce species and Brønsted acid sites,which pave the way for its practical application in the production of alkylbenzene.

关键词： Beta zeolites Catalysis Alkylation Long-chain olefins

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Enhancing thermodynamic stability of single-crystal Ni-rich cathode material via a synergistic dual-substitution strategy

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Journal of Energy Chemistry 2024年第1期88卷 428-436,I0010页

作者： Jixue Shen Hui Li Haoyu Qi Zhan Lin Zeheng Li Chuanbo Zheng Weitong Du Hao Chen Shanqing Zhang School of Metallurgy engineering Jiangsu University of Science and TechnologyZhangjiagang 215600JiangsuChina School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Guangdong laboratory of Chemistry and Fine chemical industry Jieyang Center Jieyang 515200GuangdongChina Institute of Sustainable Transformation School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006GuangdongChina Zhejiang provincial Key laboratory of advanced chemical engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Centre for Catalysis and Clean Energy School of Environment and ScienceGold Coast CampusGriffith UniversityGold Coast 4222QueenslandAustralia

Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance and safety performance or thermal stability)will restrain their wide commercial application.Herein,a single-crystal Ni-rich Li Ni_(0.83)Co_(0.12)Mn_(0.05)O_(2) cathode material is synthesized and modified by a dual-substitution strategy in which the high-valence doping element improves the structural stability by forming strong metal–oxygen binding forces,while the low-valence doping element eliminates high Li^(+)/Ni^(2+)mixing.As a result,this synergistic dual substitution can effectively suppress H2-H3 phase transition and generation of microcracks,thereby ultimately improving the thermodynamic stability of Ni-rich cathode material.Notably,the dual-doped Ni-rich cathode delivers an extremely high capacity retention of 81%after 250 cycles(vs.Li/Li+)in coin-type half cells and 87%after 1000 cycles(vs.graphite/Li^(+))in pouch-type full cells at a high temperature of 55℃.More impressively,the dual-doped sample exhibits excellent thermal stability,which demonstrates a higher thermal runaway temperature and a lower calorific value.The synergetic effects of this dual-substitution strategy pave a new pathway for addressing the critical challenges of Ni-rich cathode at high temperatures,which will significantly advance the high-energy-density and high-safety cathodes to the subsequent commercialization.

关键词： Ni-rich cathode Single crystalline Dual-substitution strategy High-temperature cathode Li-ion batteries

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Integration of morphology and electronic structure modulation on cobalt phosphide nanosheets to boost photocatalytic hydrogen evolution from ammonia borane hydrolysis

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Green Energy & Environment 2024年第2期9卷 333-343页

作者： Chao Wan Yu Liang Liu Zhou Jindou Huang Jiapei Wang Fengqiu Chen Xiaoli Zhan Dang-guo Cheng School of Chemistry and chemical engineering Anhui Province Key Laboratory of Coal Clean Conversion and High Valued UtilizationAnhui University of TechnologyMa'anshan243002China College of chemical and Biological engineering Zhejiang UniversityZhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology38 Zheda RoadHangzhou310027China Key laboratory of New Energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials&Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Nationalities University 18 Liaohe West RoadDalian116600China Institute of Zhejiang University-Quzhou 78 Jiuhua Boulevard NorthQuzhou324000China jiangsu Key laboratory of advanced Catalytic materials and Technology Changzhou University213164China

The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.

关键词： Ammonia borane Hydrogen generation Hydrolysis Cobalt phosphide nanosheets Photocatalysis

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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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Chinese Journal of chemical engineering 2024年第1期65卷 19-28页

作者： Xiaojing Liu Ruohan Zhao Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang Hebei provincial Key laboratory of Green chemical Technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Tianjin Key laboratory of chemical Process Safety Tianjin 300130China Hebei Industrial Technology Research Institute of Green chemical industry Huanghua 061100China

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词： Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen Stability

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Unveiling size-fluorescence correlation of organic nanoparticles and its use in nanoparticle size determination

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Aggregate 2024年第1期5卷 331-336页

作者： Wu-Jie Guo Shixiang Ma Hui Wang Lu Qiao Lei Chen Chenyu Hong Bin Liu Xiaoyan Zheng Hui-Qing Peng State Key laboratory of chemical Resource engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijingChina Key laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electro-photonic Conversion MaterialsKey Laboratory of Medicinal Molecule Science and Pharmaceutics Engineering of Ministry of Industry and Information TechnologySchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijingChina

Quantitatively establishing the correlation between nanoparticle size and fluorescence is essential for understanding the behavior and functionality of fluorescent nanoparticles(FNPs).However,such exploration focusing on organic FNPs has not been achieved to date.Herein,we employ the use of supramolecular polymeric FNPs prepared from tetraphenylethylene-based bis-ureidopyrimidinone monomers(bis-UPys)to relate the size to the fluorescence of organic nanoparticles.At an equal concentration of bis-UPys,a logarithmic relationship between them is built with a correlation coefficient higher than 0.96.Theoretical calculations indicate that variations in fluorescence intensity among FNPs of different sizes are attributed to the distinct molecular packing environments at the surface and within the interior of the nanoparticles.This leads to different nonradiative decay rates of the embedded and exposed bis-UPys and thereby changes the overall fluorescence quantum yield of nanoparticles due to their different specific surface areas.The established fluorescence intensity-size correlation possesses fine universality and reliability,and it is successfully utilized to estimate the sizes of other nanoparticles,including those in highly diluted dispersions of FNPs.This work paves a new way for the simple and real-time determination of nanoparticle sizes and offers an attractive paradigm to optimize nanoparticle functionalities by the size effect.

关键词： aggregation-induced emission fluorescence detection fluorescent nanoparticle nanoparticle size supramolecular polymer

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Long-range Pt-Ni dual sites boost hydrogen evolution through optimizing the adsorption configuration

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Nano Research 2024年第5期17卷 3700-3706页

作者： Cong Liu Pengfang Zhang Bing Liu Qian Meng Xuzhao Yang Yakun Li Jingli Han Yao Wang Henan Province engineering Research Center of Catalysis and Separation of Cyclohexanol College of Materials and Chemical EngineeringZhengzhou University of Light IndustryZhengzhou 450001China Shandong provincial Key laboratory of chemical Energy Storage and Novel Cell Technology Liaocheng UniversityLiaocheng 252000China Key laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringInternational Joint Research Center for Photoresponsive Molecules and MaterialsJiangnan UniversityWuxi 214122China

Elaborated design of catalytic systems with a specifically tailored site distance to match the intermediates could substantially improve reaction kinetics and boost catalytic activity under unfavorable reaction conditions.Considering the lower energy barriers of water splitting upon the synergy of dual sites,constructing synergistic Pt-M(M:transition metal)dual sites is an effective way to boost Pt with highly catalytic hydrogen evolution reaction(HER)performance.An unconventional“Ni(OH)_(2)-coated high-index Pt facets”was constructed to obtain long-range Pt-Ni dual sites,in which Ni composition as a water dissociation synergistic site can protect Pt from electrolyte corrosion and ensure efficient proton donation to Pt sites.The obtained long-range Pt-Ni dual sites present 3.84 mA·cm^(-1) of current density,which is 7.5 times specific activity higher than that of commercial Pt/C towards alkaline HER.The enhanced HER performance is attributed to synergistic catalysis on Pt-Ni dual sites accompanied by unconventional electron coupling.This work illustrates a new strategy to construct the long-range dual sites by unconventional strategy for fundamental electrocatalytic study of alkaline HER.

关键词： long-range Pt-Ni dual sites electron transfer hydrogen evolution reaction sites synergy

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