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Particuology 2024年第5期88卷 62-70页

作者： Zhuwei Gao Chengxin Li Jingjing He Zhuo Wang Xinyu Qi Lan He Shihao Wang Zhongxin Liu School of Chemical Engineering and Technology Hainan UniversityHaikou 570228China TJ-YZ School of Network Science Haikou University of EconomicsHaikou 570203China School of Food Science and Engineering Hainan UniversityHaikou 570228China key laboratory of Advanced Materials of Tropical Island Resources of Ministry of Education Hainan UniversityHaikou 570228China hainan provincial key laboratory of fine chemicals Hainan UniversityHaikou 570228China

This study aims to analyze the coking process and propose an effective method for the reutilization of fluid catalytic cracking(FCC)coke block.Herein,we analyzed the basic characteristics and chemical composition of FCC coke blocks.The results showed that the main components were carbon,oxygen,and aluminum,accounting for 60.8%,26.6%,and 11.5%,respectively.Under the conventional catalytic cracking reaction temperature from 500°C to 600°C,the formation of the first aromatic hydrocarbon was particularly important for the formation of coke.The condensation of oil-gas-entrained catalyst particles and their heavy components was the physical cause of coking,while the dehydrogenation condensation reaction of oil-gas heavy components was the chemical factor.In addition,the membrane prepared by powdered coke had excellent photothermal conversion ability,which could be heated to more than 110°C within 360 s under two fixed light intensities.The evaporation rate of photothermal water was 5.89 kg m 2 h−1,which has great industrial application potential.These works provide a novel and effective method of separation membrane for the reutilization of FCC coke blocks.

关键词： Coking process Reutilization of FCC coke Carbonaceous deposition Membrane Photothermal conversion

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

Recent advances in multifunctional shape memory photonic crystals and practical applications

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Nano Research 2024年第1期17卷 79-96页

作者： Yong Qi Shufen Zhang State key laboratory of fine chemicals Frontier Science Center for Smart MaterialsDalian University of TechnologyDalian 116024China

Shape memory photonic crystals(SMPCs)are smart composite materials with changeable structural color integrated by shape memory polymer and photonic crystals.SMPC can produce one or more temporary shapes through nanoscale deformation,memorizing current states.SMPC can be recovered to their original shapes or some intermediate states under external stimuli,accompanied by the variation of structural color.As porous carriers with built-in sensing properties,SMPCs promoted the interdisciplinary development of nanophotonic technology in materials science,environmental engineering,biomedicine,chemical engineering,and mechanics.Herein,the recent progress on multifunctional SMPCs and practical applications,including traditional and cold programmable SMPCs,is summarized and discussed.The primary concern is shape programming at the nanoscale that has demonstrated numerous attractive functions,including smart sensing,ink-free printing,solvent detection,reprogrammable gradient wetting,and controllable bubble transportation,under variations of the surface nanostructure.It aims to figure out the nanoscale shape memory effects on structural color conversion and additional performance,inspiring the fabrication of the next generation of SMPCs.Finally,perspectives on future research directions and applications are also presented.It is believed that multifunctional SMPCs are powerful nanophotonic tools for the interdisciplinary development of numerous disciplines in the future.

关键词： photonic crystal shape memory structural color cold programmable shape recovery

Multiresponsive,easy-reversible,and dual-visual Pt(Ⅱ)salt nanostructures for advanced anti-counterfeiting application

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Nano Research 2024年第1期17卷 372-381页

作者： Zhen Su§ Depeng Li§ Lixin Zhang Si Tian Yuhong Su Xiaoyun Hu Duan Xiong Qingqing Guan key laboratory of Oil and Gas fine chemicals Ministry of Education College of Chemical EngineeringXinjiang UniversityUrumqi 830017China

Smart materials that integrate multi-stimuli response,full reversibility,and dual-visual read-out channel are highly desired for anticounterfeiting and information encryption applications.Herein,we developed a multiresponsive perchlorate terpyridyl Pt(Ⅱ)nano complex which could undergo fully reversible conversion between three forms stimulated by water or formaldehyde molecule due to the extent of Pt–Pt interaction.Meanwhile,a dual-visual channel,i.e.,the colorimetric channel changed from yellow to orange or red and the corresponding luminescent channel from orange to orange-red or red,has also been found.The weak and equivalent strength of ion-dipole interaction and hydrogen bond that generated between formaldehyde/water and Pt(II)salt result in the easy-control reversibility between the three forms.Furthermore,by introducing different polymer matrices,1Cl·ClO_(4)@PMMA(1Cl·ClO_(4):[Pt(tpy)Cl]·ClO4,tpy:2,2':6',2''-terpyridine),PMMA:poly(methyl methacrylate))and 1Cl·ClO4@PVA(PVA:polyvinyl alcohol)are successfully constructed,which exhibit different reversible behaviors since the PMMA and PVA matrix exert different influences on the strength of hydrogen-bond.Those smart Pt(II)salt nanostructures present great potential for high-security-level anticounterfeiting application.

关键词： Pt(II)complex multiresponse reversibility anticounterfeiting information encryption

Avoiding Sabatier's limitation through pulsed electrocatalysis for enhanced nitrogen oxidation performance

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Journal of Energy Chemistry 2024年第8期95卷 484-489页

作者： Xiping Guan Zhongfen Nie Linlin Zhang Mingxia Guo Chuanwei Shi Chunlei Gu Xia Liu Xin Ding College of Chemistry and Chemical Engineering Qingdao University State key laboratory of fine chemicals Dalian University of Technology(DUT)

1. Introduction The activation and conversion of the Earth’s abundant inert nitrogen resources into high-value-added products epitomize one of nature’s most critical processes[1–3]. Nitric acid （HNO3）, as a pivotal industrial raw material, showcases an extensive range of applications and possesses substantial economic value in the production of indispensable chemical compounds[4–6]. Currently,

关键词： AMMONIA

Asymmetrically ligated single atomic nickel sites for efficient hydrogen peroxide electrosynthesis

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Nano Research 2024年第3期17卷 1094-1100页

作者： Xusheng Cheng Jinwen Hu Wenzhe Shang Jingya Guo Cuncun Xin Songlin Zhang Suchan Song Wei Liu Yantao Shi State key laboratory of fine chemicals Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024China

Atomic transition-metal-nitrogen-carbon electrocatalysts hold great promise as alternatives to benchmark Pt in the oxygen reduction reaction.The pristine metal centers with quasi square-planar D_(4h) configuration,however,still suffer from unfavorable energetics and thereby strong activity/selectivity trade-off during the catalytic process.Here we present a ligand-field engineering of single-atom Ni-N-C catalysts to boost the sluggish kinetics via rationally constructing prototypical asymmetrically ligated Ni-N_(3)O_(1) sites.The as-obtained Ni-supported multi-walled carbon nanotubes with molten salt-treated(defined as Ni/CNS)catalyst delivered an excellent H_(2)O_(2) selectivity(>90%)within a wide potential window(0.2–0.7 V vs.reversible hydrogen electrode(RHE))and robust stability(for 10 h)in alkaline medium.Combined electron paramagnetic resonance and theoretical analysis rationalize this finding and demonstrate that the broken symmetry facilitates the electron transfer of a σ* to O–O orbital as compared to the Ni-N_(4) counterpart,playing an indispensable role in efficient O_(2) activation.

关键词： broken D4h single nickel sites oxygen reduction H_(2)O_(2)production

Discovery and structure-activity relationship studies of novel tetrahydro-β-carboline derivatives as apoptosis initiators for treating bacterial infections

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Journal of Integrative Agriculture 2024年第4期23卷 1259-1273页

作者： Shanshan Su Hongwu Liu Junrong Zhang Puying Qi Yue Ding Ling Zhang Linli Yang Liwei Liu Xiang Zhou Song Yang National key laboratory of Green Pesticide/key laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education/Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025China

Developing and excavating new agrochemicals with highly active and safe is an important tactic for protecting crop health and food safety.In this paper,to discover the new bactericide candidates,we designed,prepared a new type of1,2,3,4-tetrahydro-β-carboline(THC)derivatives and evaluated the in vitro and in vivo bioactivities against the Xanthomonas oryzae pv.oryzae(Xoo),Xanthomonas axonopodis pv.citri(Xac),and Pseudomonas syringae pv.actinidiae(Psa).The in vitro bioassay results exhibited that most title molecules possessed good activity toward the three plant pathogenic bacteria,the compound A17 showed the most active against Xoo and Xac with EC50 values of 7.27 and 4.89 mg mL^(-1)respectively,and compound A8 exhibited the best inhibitory activity against Psa with EC50value of 4.87 mg mL^(-1).Pot experiments showed that compound A17 exhibited excellent in vivo antibacterial activities to manage rice bacterial leaf blight and citrus bacterial canker,with protective efficiencies of 52.67 and 79.79%at 200 mgmL^(-1),respectively.Meanwhile,compound A8 showed good control efficiency(84.31%)against kiwifruit bacterial canker at 200 mg mL^(-1).Antibacterial mechanism suggested that these compounds could interfere with the balance of the redox system,damage the cell membrane,and induce the apoptosis of Xoo cells.Taken together,our study revealed that tetrahydro-β-carboline derivatives could be a promising candidate model for novel broadspectrum bactericides.

关键词： tetrahydro-β-carboline derivatives antibacterial activity ROS cell apoptosis

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Bactericidal bissulfone B7 targets bacterial pyruvate kinase to impair bacterial biology and pathogenicity in plants

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Science China(Life Sciences) 2024年第2期67卷 391-402页

作者： Awei Zhang Haizhen Zhang Ronghua Wang Hongfu He Baoan Song Runjiang Song National key laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationCenter for R&D of Fine Chemicals of Guizhou UniversityGuiyang 550025China

The prevention and control of rice bacterial leaf blight(BLB)disease has not yet been achieved due to the lack of effective agrochemicals and available targets.Herein,we develop a series of novel bissulfones and a novel target with a unique mechanism to address this challenge.The developed bissulfones can control Xanthomonas oryzae pv.oryzae(Xoo),and 2-(bis(methylsulfonyl)methylene)-N-(4-chlorophenyl)hydrazine-1-carboxamide(B_(7))is more effective than the commercial drugs thiodiazole copper(TC)and bismerthiazol(BT).Pyruvate kinase(PYK)in Xoo has been identified for the first time as the target protein of our bissulfone B_(7).PYK modulates bacterial virulence via a CRP-like protein(Clp)/two-component system regulatory protein(reg R)axis.The elucidation of this pathway facilitates the use of B_(7)to reduce PYK expression at the transcriptional level,block PYK activity at the protein level,and impair the interaction within the PYK-Clp-reg R complex via competitive inhibition,thereby attenuating bacterial biology and pathogenicity.This study offers insights into the molecular and mechanistic aspects underlying anti-Xoo strategies that target PYK.We believe that these valuable discoveries will be used for bacterial disease control in the future.

关键词： 2-bissulfone-N-phenylhydrazine-1-carboxamide derivatives Xoo antibacterial activities pyruvate kinase regulatory mechanism

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In-situ Generation of Hydroxyl Layers in Coo@FeSe_(2) Catalyst for High Selectivity Seawater Electrolysis

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Chinese Journal of Chemistry 2024年第1期42卷 48-54,I0004页

作者： Suyang Feng Peng Rao Xiao Wu Ke Li Anyuan Qi Yanhui Yu Jing Li Peilin Deng Yuliang Yuan Shaolei Wang Xinlong Tian Zhenye Kang State key laboratoryof Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchoolof Chemical Engineering andTechnologyHainan UniversityHaikouHainan 570228China key Laboraory of Polyoxmetalate andReticular Material Chemtry of Ministy of Education School of Chmistry Northeast NormalUniversity ChangchunJilin 130024China National Energy Group Ledong Power Generation Co. Ltd.LedongHainan 572539China

Seawater electrolysis holds great promise for hydrogen production in the future,while the development of anodic catalysts has been severely hampered by the side-reaction,chloride evolution reaction.In this work,nano-flower-cluster structured Coo@FeSe_(2)/CF catalysts are synthesized via a scalable electrodeposition technique,and the performance is systematically studied.The oxygen evolution reaction(OER)overpotential of Co0@FeSe_(2)/CF is 267 mV at 100 mA.cm^(-2),which is significantly lower than that of the IrO_(2) catalyst(435 mV).Additionally,the catalyst shows high selectivity for OER(97.9%)and almost no loss of activity after a durability test for 1100 h.The impressive performance is attributed to the dense rod-like structure with abundant active centers after electrochemical activation and the in-situ generated CoOOH and FeOOH that improve the catalytic activity of the catalyst.The synergistic effect induced bythenon-uniform structureendows the catalyst with excellent stability.

关键词： Energy Transfer Seawat erelectrolysis Oxygen evolution reaction Electrodeposition method CoO@FeSe_(2)/CF catalyst Nano-flower-cluster structure Catalytic activity

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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