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experimental and theoretical investigation of sulfur-doped g-C_(3)n_(4)nanosheets/FeCo_(2)O_(4)nanorods s-scheme heterojunction for photocatalytic H_(2)evolution

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nano Research 2024年第9期17卷 8007-8016页

作者： Haitao Wang Lianglang Yu Jiahe Peng Jing Zou Weiping Gong Jizhou Jiang school of Chemistry and Environmental Engineering School of Environmental Ecology and Biological EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Guangdong Provincial Key laboratory for Electronic Functional Materials and Devices Huizhou UniversityHuizhou 516007China

g-C_(3)n_(4)emerges as a promising metal-free semiconductor photocatalyst due to its cost-effectiveness,facile synthesis,suitable visible light response,and robust thermal ***,its practical application in photocatalytic hydrogen evolution reaction(HER)is impeded by rapid carrier recombination and limited light absorption *** this study,we successfully develop a novel g-C_(3)n_(4)-based step-scheme(s-scheme)heterojunction comprising two-dimensional(2D)sulfur-doped g-C_(3)n_(4)nanosheets(sCn)and one-dimensional(1D)FeCo_(2)O_(4)nanorods(FeCo_(2)O_(4)),demonstrating enhanced photocatalytic HER *** engineered sCn/FeCo_(2)O_(4)s-scheme heterojunction features a well-defined 2D/1D heterogeneous interface facilitating directed interfacial electron transfer from FeCo_(2)O_(4)to sCn,driven by the lower Fermi level of sCn compared to FeCo_(2)O_(4).This establishment of electron-interacting 2D/1D s-scheme heterojunction not only facilitates the separation and migration of photogenerated carriers,but also enhances visible-light absorption and mitigates electron-hole pair *** structure analysis and density functional theory calculations corroborate that the carrier migration in the sCn/FeCo_(2)O_(4)photocatalyst adheres to a typical s-scheme heterojunction mechanism,effectively retaining highly reactive photogenerated ***,the optimized sCn/FeCo_(2)O_(4)heterojunction exhibits a substantially high hydrogen production rate of 6303.5μmol·g^(-1)·h^(-1)under visible light excitation,which is 2.4 times higher than that of the ***,the conjecture of the s-scheme mechanism is confirmed by in situ XPs *** 2D/1D s-scheme heterojunction established in this study provides valuable insights into the development of high-efficiency carbon-based catalysts for diverse energy conversion and storage applications.

关键词： g-C_(3)n_(4) FeCo_(2)O_(4) s-scheme heterojunction photocatalytic hydrogen evolution reaction(HER)

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n-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies

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Journal of Zhejiang University-science A(Applied Physics & Engineering) 2024年第4期25卷 340-356页

作者： Yong GUO Mengxia CHEn Ting CHEn Ying GUO Zixuan XU Guowei XU soukthakhane sInsOnEsACK Keophoungeun KAnMAnY Key laboratory of Integrated Regulation and Resource Development on shallow Lakes Ministry of EducationCollege of EnvironmentHohai UniversityNanjing 210093China Key laboratory of Environmental Engineering of Jiangsu Province Jiangsu Provincial Academy of Environmental ScienceNanjing 210036China state Key laboratory of Pollution Control and Resource Reuse Nanjing UniversityNanjing 210023China Central Environmental laboratory Natural Resources and Environment Research InstituteMinistry of Natural Resources and EnvironmentVientiane 999012Laos

We investigated the influence mechanism of n-doping for dissolved black carbon(DBC)photodegradation of organic *** degradation performance of n-doped dissolved black carbon(nDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under *** levels are both better than DBC degradation performances for TC(68%)and MB(18%)under *** species quenching experiments suggest that h and-O,are the main reactive species for nDBC photodegraded TC,while-OH and h*are the main reactive species for nDBC photodegraded MB.-OH is not observed during DBC photodegradation of *** is likely because n-doping increases valence-band(VB)energy from 1.55 eV in DBC to 2.04 eV in nDBC;the latter is strong enough to oxidize water to ***,n-doping increases the DBC band gap of 2.29 to 2.62 eV in nDBC,resulting in a higher separation efficiency of photo-generated electrons-holes in nDBC than in *** these factors give nDBC stronger photodegradation performance for TC and MB than ***-performance liquid chromatography-mass spectrometry(HPLC-Ms)characterization and toxicity evaluation with the quantitative structure-activity relationship(QsAR)method suggest that TC photodegradation intermediates produced by nDBC have less aromatic structure and are less toxic than those produced by *** adopted a theoretical approach to clarify the relationship between the surface groups of nDBC and the photoactive species *** results add to the understanding of the photochemical behavior of nDBC.

关键词： Dissolved black carbon(DBC) n-doping Organic pollutants Band gap Photodegradation

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Tuning interface mechanism of FeCo alloy embedded n,s-codoped carbon substrate for rechargeable Zn-air battery

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Journal of Energy Chemistry 2024年第6期93卷 400-410,I0010页

作者： Hui Chang Lulu Zhao shan Zhao Zong-Lin Liu Peng-Fei Wang Ying Xie Ting-Feng Yi school of Materials science and Engineering Northeastern UniversityShenyang 110819LiaoningChina Key laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina Key laboratory of Dielectric and Electrolyte Functional Material Hebei Province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004HebeiChina

The interface mechanism between catalyst and carbon substrate has been the focus of *** this paper,the FeCo alloy embedded n,s co-doped carbon substrate bifunctional catalyst(FeCo/s-nC)is obtained by a simple one-step pyrolysis *** experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of s atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon *** FeCo/snC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/s-nC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for *** addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/s-nC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle *** results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.

关键词： FeCo alloy n s co-doped carbon DFT calculation Zn-air batteries Interfacial interaction

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Crystallinity-defect matching relationship of g-C_(3)n_(4): experimental and theoretical perspectives

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Green Energy & Environment 2024年第4期9卷 623-658页

作者： Yuhan Li Ziteng Ren Zhengjiang He Ping Ouyang Youyu Duan Wendong Zhang Kangle Lv Fan Dong Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Key Laboratory of Catalysis and New Environmental MaterialsChongqing Technology and Business UniversityChongqing400067China nanchang Institute of Technology Nanchang33044China Key laboratory of Resources Conversion and Pollution Control of the state Ethnic Affairs Commission College of Resources and Environmental ScienceSouth-Central Minzu UniversityWuhan430074China College of Physics and Center of Quantum Materials and Devices Chongqing UniversityChongqing401331China Chongqing Key laboratory of Green synthesis and Application Chongqing Normal UniversityChongqing401331China

Good crystallinity can reduce the charge recombination centers caused by defects,whilst structures with strong polycondensation have high charge mobility,leading to more charge transfer to the material surface for *** effort has been put into the preparation of a highly efficient g-C_(3)n_(4) with defects to improve its application potential under the premise in high ***,this review paper emphasizes the importance to balance the defect and crystallinity of g-C_(3)n_(4).In addition,detailed discussion on the relationship between defects and activity of g-C_(3)n_(4) was carried out based on its applications in environmental purification(e.g.,VOCs oxidation,nO_(x) oxidation,H_(2)O_(2) evolution,sterilization,pesticide oxidation)and energy conversion(H_(2) evolution,n_(2) fixation and CO_(2) reduction).Lastly,the challenge in developing more efficient defective g-C_(3)n_(4) photocatalytic materials is summarized.

关键词： Photocatalysis Defect G-C_(3)n_(4) Crystallinity Application

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experimental study on Impingement Processes of Fuel sprays on Biomimetic structured surfaces

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Journal of Bionic Engineering 2024年第1期21卷 362-373页

作者： Yanling Chen Liang Guo Wanchen sun Yuying Yan Rong Xuan Junfeng Zhang state Key laboratory of Automotive simulation and Control Jilin UniversityChangchun 130025China Faculty of Engineering University of NottinghamNottingham NG72RDUK

To improve the controllability of the wall-wetting process after the fuel spray-wall impingement in internal combustion engines,the methods of laser etching,chemical etching and surface free energy modification are used to prepare biomimetic structured surfaces with different *** impingement processes of diesel and n-butanol sprays on the walls under different conditions are experimentally *** the surface oleophilicity increases,the spreading radius of wall-impinging sprays *** about 5 s after the fuel injections,the fuel spray droplets hit the walls for the first time,and the secondary breakup and rebound *** mixture concentrations of different fuels hitting the various walls reach the peak *** a higher surface temperature,the peak value of the mixture concentration is mainly related to the heat flux to the fuel droplets in different boiling regimes from the metal *** concentration of the air–fuel mixture in the near wall region increases with increasing surface oleophilicity,increasing wall temperature and decreasing ambient *** with diesel,n-butanol presents a higher air–fuel mixture concentration in the near wall region.

关键词： spray-wall impingement Morphological development Air-fuel mixture concentration surface wettability Wall temperature:Ambient pressure

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Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics:A combined experimental and theoretical study

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Chinese Chemical Letters 2024年第8期35卷 514-519页

作者： Longlong Geng Huiling Liu Wenfeng Zhou Yong-Zheng Zhang Hongliang Huang Da-shuai Zhang Hui Hu Chao Lv Xiuling Zhang suijun Liu shandong Provincial Key laboratory of Monocrystalline silicon semiconductor Materials and Technology College of Chemistry and Chemical EngineeringDezhou UniversityDezhou 253023China school of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255000China state Key laboratory of separation Membranes and Membrane Processes School of Chemical Engineering and TechnologyTiangong UniversityTianjin 300387China school of Chemistry and Chemical Engineering Jiangxi Provincial Key Laboratory of Functional Molecular Materials ChemistryJiangxi University of Science and TechnologyGanzhou 341000China

Metal-organic frameworks(MOFs)functionalized with open metal sites(OMss)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest ***,rational tailoring of the coordination environment of metal nodes dur-ing the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with ***,we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ)sites,namely[Cu(HCOO)(pzta)]_(n)(HL-1),{[Cu(PTA)0.5(pzta)(H_(2)O)]·2H_(2)O}_(n)(HL-2)and[Cu(nA)0.5(pzta)]_(n)(HL-3)(Hpzta=3-pyrazinyl-1,2,4-triazole;PTA=terephthalic acid;nA=1,4-naphthalene dicarboxylic acid),based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ***-markably,the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions(25℃and 1 atm).In particular,the complete conversion of 4-nitrophenol(4-nP)took only 30 s on HL-2,reaching a record-high TOF value compared with previously reported metal *** combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron trans-port between the substrates,and was responsible for the outstanding *** work shined lights on the further enhancement of performance for MOFs through rational OMss construction.

关键词： Metal-organic frameworks Open metal sites Catalysis Copper node 4-nitrophenol

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A cascade of in situ conversion of bicarbonate to CO_(2) and CO_(2) electroreduction in a flow cell with a ni-n-s catalyst

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Journal of Energy Chemistry 2024年第1期88卷 183-193,I0005页

作者： Linghui Kong Min Wang Yongxiao Tuo shanshan Zhou Jinxiu Wang Guangbo Liu Xuejing Cui Jiali Wang Luhua Jiang nanomaterials and Electrocatalysis laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina state Key laboratory of Heavy Oil Processing College of New EnergyChina University of Petroleum(East China)Qingdao 266580ShandongChina

Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high *** electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode ***,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow *** a tailored ni-n-s single atom catalyst(sACs),where sulfur(s)atoms located in the second shell of ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is *** experimental results and density functional theory(DFT)calculations reveal that the introduction of s increases the p electron density of n atoms near ni atom,thereby stabilizing^(*)H over n and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)*** a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported ni *** importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid *** work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.

关键词： s doped ni-n-C single atom catalysts CO_(2)electrochemical reduction DFT calculations Membrane electrode assembly Reduction of bicarbonate

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experimental determination of the Young’s modulus of individual single-walled carbon nanotubes with single chirality

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nano Research 2024年第8期17卷 7522-7532页

作者： Jianlin sun Xiao Zhang Yanchun Wang Mingming Li Xiaojun Wei Huaping Liu Weiya Zhou Beijing national laboratory for Condensed Matter Physics and Institute of PhysicsChinese Academy of SciencesBeijing 100190China school of Physical sciences and College of Materials science and Optoelectronic Technology University of Chinese Academy of SciencesBeijing 100049China songshan Lake Materials laboratory Dongguan 523808China Beijing Key laboratory for Advanced Functional Materials and structure Research Beijing 100190China

One-dimensional carbon nanotube(CnT)exhibits excellent mechanical properties and is considered to be an ideal candidate material for the space ***,subtle changes in its chirality strongly affect its physical and chemical properties,including mechanical properties(such as Young's modulus,YM).Theoretical studies reveal that the YMs of perfect single-walled carbon nanotubes(sWCnTs)are in the order of TPa and related to their ***,due to the lack of sWCnTs samples with well-defined structures and the difficulties in mechanical tests on individual sWCnTs,the theoretical correlations between YM and structure of sWCnTs have not been verified and are still in debate,which directly influences the practical utilization of the excellent mechanical properties of *** this work,we have developed an experimental method to measure the YM of an individual micrometer-scale suspended CnT by atomic force microscopy.A distinct regularity is found between the YM and chirality(i.e.,chiral angle and diameter)of sWCnT in the experiment for the first *** comparing the YMs of sWCnTs with similar diameters and different chiral angles,it manifests that the sWCnT with a near zigzag configuration has a larger *** finding suggests that the effect of sWCnT’s structures on the YMs cannot be *** developed method of measuring YMs of sWCnTs will be valuable for further experimental research on the inherent physical and chemical properties of sWCnTs.

关键词： Young's modulus single-walled carbon nanotubes single chirality atomic force microscopy

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Impact of H_(2)s on Hg^(0)capture performance over nitrogen-doped carbon microsphere sorbent:experimental and theoretical insights

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Frontiers of Chemical science and Engineering 2024年第3期18卷 89-100页

作者： Guopei Zhang Xiaoyang Zhang Xiangwen Xing Xiangru Kong Lin Cui Dong Yong national Engineering laboratory for Reducing Emissions from Coal Combustion Shandong UniversityJinan250061China Bingtuan Energy Development Institute Shihezi UniversityShihezi832000China

A nitrogen-doped carbon microsphere sorbent with a hierarchical porous structure was synthesized via aggregation-hydrothermal *** Hg^(0)adsorption performance of the nitrogen-doped carbon microsphere sorbent was tested and compared with that of the coconut shell activated carbon prepared in the *** effect of H_(2)s on Hg^(0)adsorption was also *** nitrogen-doped carbon microsphere sorbent exhibited superior mercury removal performance compared with that of coconut shell activated *** the absence of H_(2)s at a low temperature(≤100℃),the Hg^(0)removal efficiency of the nitrogen-doped carbon microsphere sorbent exceeded 90%.This value is significantly higher than that of coconut shell activated carbon,which is approximately 45%.H_(2)s significantly enhanced the Hg^(0)removal performance of the nitrogen-doped carbon microsphere sorbent at higher temperatures(100–180℃).The hierarchical porous structure facilitated the diffusion and adsorption of H_(2)s and Hg^(0),while the nitrogen-containing active sites significantly improved the adsorption and dissociation capabilities of H_(2)s,contributing to the generation of more active sulfur species on the surface of the nitrogen-doped carbon microsphere *** formation of active sulfur species and Hgs on the sorbent surface was further confirmed using X-ray photoelectron spectroscopy and Hg^(0)temperature-programmed desorption *** functional theory was employed to elucidate the adsorption and transformation of Hg^(0)on the sorbent surface.H_(2)s adsorbed and dissociated on the sorbent surface,generating active sulfur species that reacted with gaseous Hg^(0)to form Hgs.

关键词： nitrogen-doped carbon microsphere H_(2)s Hg^(0)removal adsorption mechanism

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Mycorrhizal fungi mitigate nitrogen losses of an experimental grassland by facilitating plant uptake and soil microbial immobilization

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Pedosphere 2024年第2期34卷 399-410页

作者： Yangyang JIA Marcel G.A.VAn DER HEIJDEn Alain Y.VALZAnO-HELD Markus JOCHER Florian WALDER Postdoctoral Mobile station of Ecology College of Ecology and EnvironmentXinjiang UniversityÜrümqi 830046China Research Group Plant-soil Interactions AgroscopeZürich 8046Switzerland Research Group Climate and Agriculture AgroscopeZürich 8046Switzerland Department of Plant and Microbial Biology University of ZürichZürich 8008Switzerland Research Group soil Quality and soil Use AgroscopeZürich 8046Switzerland

nitrogen(n)is one of the most limited nutrients of terrestrial ecosystems,whose losses are prevented in tightly coupled cycles in finely tuned *** change-induced n enrichment through atmospheric deposition and application of vast amounts of fertilizer are now challenging the terrestrial n *** mycorrhizal fungi(AMF)are known drivers of plant-soil nutrient fluxes,but a comprehensive assessment of AMF involvement in n cycling under global change is still ***,we simulated n enrichment by fertilization(low/high)in experimental grassland microcosms under greenhouse conditions in the presence or absence of AMF and continuously monitored different n pathways over nine *** found that high n enrichment by fertilization decreased the relative abundance of legumes and the plant species dominating the plant community changed from grasses to forbs in the presence of AMF,based on aboveground *** presence of AMF always maintained plant n:phosphorus(P)ratios between 14 and 16,no matter how the soil n availability *** in plant n:P ratios due to the increased plant n and P uptake might thus be a primary pathway of AMF altering plant community ***,we constructed a comprehensive picture of AMF’s role in n cycling,highlighting that AMF reduced n losses primarily by mitigating n leaching,while n_(2)O emissions played a marginal *** mycorrhizal fungi reduced n_(2)O emissions directly through the promotion of n_(2)O-consuming *** underlying mechanism for reducing n leaching is mainly the AMF-mediated improved nutrient uptake and AMF-associated microbial *** results indicate that synergies between AMF and other soil microorganisms cannot be ignored in n cycling and that the integral role of AMF in n cycling terrestrial ecosystems can buffer the upcoming global changes.

关键词： n cycling n enrichment n uptake n:P ratio plant community structure symbiotic soil fungi

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