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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 pollutants.The degradation performance of n-doped dissolved black carbon(nDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under irradiation.These levels are both better than DBC degradation performances for TC(68%)and MB(18%)under irradiation.Reactive 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 MB.This 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 form-OH.Additionally,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 DBC.AIl these factors give nDBC stronger photodegradation performance for TC and MB than DBC.High-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 DBC.We adopted a theoretical approach to clarify the relationship between the surface groups of nDBC and the photoactive species produced.Our 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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Effect of N-doping-derived solvent adsorption on electrochemical double layer structure and performance of porous carbon

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Journal of Energy Chemistry 2023年第5期80卷 120-127,I0004页

作者： Zhe-Fan Wang Cheng Tang Qian Sun Ya-Lu Han Zhi-Jian Wang Lijing Xie Shou-Chun Zhang Fang-Yuan Su Cheng-Meng Chen CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina University of Chinese Academy of Sciences Bejing 100049China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBejing 100084Chind

n-doped porous carbon has been extensively investigated for broad electrochemical applications.The performance is significantly impacted by the electrochemical double layer(EDL),which is material dependent and hard to characterize.Limited understanding of doping-derived EDL structure hinders insight into the structure-performance relations and the rational design of high-performance materials.Thus,we analyzed the mass and chemical composition variation of EDL within electrochemical operation by electrochemical quartz crystal microbalance,in-situ X-ray photoelectron spectroscopy,and time-offlight secondary ion mass spectrometry.We found that N-doping triggers specifically adsorbed propylene carbonate solvent in the inner Helmholtz plane(IHP),which prevents ion rearrangement and enhances the migration of cations.However,this specific adsorption accelerated solvent decomposition,rendering rapid performance degradation in practical devices.This work reveals that the surface chemistry of electrodes can cause specific adsorption of solvents and change the EDL structure,which complements the classical EDL theory and provide guidance for practical applications.

关键词： Carbon materials Electrochemical double layer Electrochemical quartz crystal microbalance In-situ X-ray photoelectron spectroscopy N-doping

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Synergistic effect of lithiophilic Zn nanoparticles and N-doping for stable Li metal anodes

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Journal of Energy Chemistry 2022年第2期31卷 439-447页

作者： Lei You Shunlong Ju Jianwen Liu Guanglin Xia Zaiping Guo Xuebin Yu Department of Materials Science Fudan UniversityShanghai 200433China Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry-of-Education Key Laboratory for Synthesis and Applications of Organic Functional MoleculesCollege of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062HubeiChina School of Chemical Engineering&Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Li metal is the most ideal anode material for next-generation high energy lithium-ion batteries.The uncontrollable growth of Li dendrites,however,hinders its practical application.Herein,we propose the adoption of Zn nanoparticles uniformly embedded in n-doped carbon polyhedra homogeneously built on carbon cloth(Zn@nC@CC)to prevent the formation of Li dendrites.Based on theoretical calculation and experimental observation,lithiophilic Zn nanoparticles and N-doping inside of the assynthesized Zn@nC play a synergistic role in enhancing the adsorption capacity with Li,thus resulting in uniform Li deposition and complete suppression of Li dendrites.Moreover,the porous n-doped carbon polyhedras uniformly distributed on carbon cloth effectively relieves the volume change of Li upon repeated Li stripping/plating process,which contributes to preserving the structural integrity of the whole electrode and hence enhancing its long-term cycling stability.Benefiting from these synergistic effects,the Li-Zn@nC@CC electrode delivers a prolonged lifespan of over 1200 h at 1 mA cm^(-2) with an areal capacity of 1 mA h cm^(-2) in symmetric cells and high Coulombic efficiencies of 95.4%under an ultrahigh capacity of 12 mA h cm^(-2).Remarkably,Li-Zn@nC@CC//LiFePO_(4) full cells deliver a high reversible capacity of 110.2 mA h g^(-1) at 1 C over 200 cycles.

关键词： Li metal anodes Zn nanoparticles N-doping Synergistic effect

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Influence of N-doping on dielectric properties of carbon-coated copper nanocomposites in the microwave and terahertz ranges

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Journal of Materiomics 2022年第6期8卷 1131-1140页

作者： Feirong Huang Shuting Fan Yuqi Tian Xinghao Qu Xiyang Li MaoFan Qin Javid Muhammad Xuefeng Zhang Zhidong Zhang Xinglong Dong Key Laboratory of Materials Modification by Laser Ion and Electron Beams(Ministry of Education)School of Materials Science and EngineeringDalian University of TechnologyDalian116024China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen518060China Institute of Advanced Magnetic Materials College of Materials and Environmental EngineeringHangzhou Dianzi UniversityHangzhou110819China Shenyang national Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang110015China

Carbon-coated Cu nanocomposites (Cu@C nCs) consisting of core-shell nanoparticles and nanorods weresynthesized by arc discharge plasma under an atmosphere of He and H_(2) gas, and the N-doping of themwas achieved by a post-treatment process using ureal as the precursor. The concentration of n in the ndoped samples varies in the range of 0.62%-2.31 % (in mole), with a transformation from pyrrolic n tographitic n when increasing the relative content of ureal. Dielectric properties of the nCs without or withN-doping in the microwave and THz bands were investigated. The n-doped samples achieve theenhanced dielectric loss in both microwave and THz bands. In the microwave band, dielectric loss wasdominated by interfacial polarization, dipolar polarization, and conduction loss, while in the THz band,plasma resonance, ionic polarization and conduction loss are responsible for the dielectric loss, with astrong absorption characteristic dominated by conductive effect.

关键词： Cu/C nanocomposite Dielectric property N-doping Terahertz frequency

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氢键调控实现高稳定性、高迁移率和高n-掺杂效率的菲咯啉类电子传输材料

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Science Bulletin 2020年第2期65卷 153-160,88页

作者：宾正杨史棣元苏蓉川憨卫国张东东段炼 Key Laboratory of Organic Optoelectronics and Department of Chemistry Tsinghua UniversityBeijing 100084China College of Chemistry Sichuan UniversityChengdu 610064China Center for Flexible Electronics Technology Tsinghua UniversityBeijing 100084China

4,7-二苯基-1,10-菲咯啉(BPhen)是一种常用的电子传输材料,凭借其电子迁移率高、制备工艺简单等优点,在有机电致发光二极管(OLED)中得到广泛的应用.然而,其较低的玻璃化转变温度(Tg)导致器件稳定性差,严重制约其进一步发展和应用.本文... 详细信息

4,7-二苯基-1,10-菲咯啉(BPhen)是一种常用的电子传输材料,凭借其电子迁移率高、制备工艺简单等优点,在有机电致发光二极管(OLED)中得到广泛的应用.然而,其较低的玻璃化转变温度(Tg)导致器件稳定性差,严重制约其进一步发展和应用.本文通过分子间氢键作用的调控,在菲咯啉衍生物中同时实现了高的热稳定性(Tg=111.9℃)和大的电子迁移率(7.8×10-4 cm2/(Vs)),并且可以活化惰性金属实现非常优异的n型掺杂性能,显著降低OLED器件驱动电压,提高OLED器件效率和改善OLED器件稳定性.

关键词： Phenanthroline Electron transport material N-doping Exciplex Organic light-emitting diodes

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Direct electrochemical N-doping to carbon paper in molten LiCl-KCl-Li3n

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International Journal of Minerals,Metallurgy and Materials 2020年第12期27卷 1687-1694页

作者： Dong-hua Tian Zhen-chao Han Ming-yong Wang Shu-qiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

Graphite materials are widely used as electrode materials for electrochemical energy storage.N-doping is an effective method for enhancing the electrochemical properties of graphite.A novel one-step N-doping method for complete and compact carbon paper was proposed for molten salt electrolysis in the Li Cl-KCl-Li3 n system.The results show that the degree of graphitization of carbon paper can be improved by the electrolysis of molten salts,especially at 2.0 V.nitrogen gas was produced at the anode and nitrogen atoms can substitute carbon atoms of carbon paper at different sites to create nitrogen doping during the electrolysis process.The doping content of n in carbon paper is up to 13.0 wt%.There were three groups of nitrogen atoms,i.***.quaternary n(n-Q),pyrrolic n(n-5),and pyridinic n(n-6)in N-doping carbon paper.N-doping carbon paper as an Al-ion battery cathode shows strong charge-recharge properties.

关键词： N-doping carbon paper molten salt electrolysis electrochemical process

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Diameter dependent doping in horizontally aligned high-density n-doped SWnT arrays

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nano Research 2019年第8期12卷 1845-1850页

作者： Pan Li Yiming Li Xiao Zhang Jun Chen Yingwen Cheng Yi Li Yanwen Ma Jie Liu Key Laboratory for Organic Electronics and Information Displays Jiangsu Key Laboratory for BiosensorsInstitute of Advanced Materials (LAM)Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM)Nanjing University of Posts & Telecommunications9 Wenyuan RoadNanjing 210023China Department of Chemistry Duke UniversityDurhamNorth Carolina 27708USA Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIllinois 60115USA

We reported the growth of horizontally aligned nitrogen-doped single-walled carbon nanotubes (SWnTs) on quartz substrates. The synthesized SWnTs were comprehensively characterized at the single nanotube level. Owing to the highly aligned nature of the nanotubes, we were able to investigate the diameter dependent doping mechanism through systematic resonant Raman spectroscopy studies. Other than the formerly found narrowing effect by N-doping, we proposed that the nanotube diameter affects the introduction of n atoms into the carbon lattice in an elaborate way. The obtained doping level increased along with the nanotube diameter but lost the increasing trend when the diameter became larger and experienced a slight decrease after reaching the local peak value. These insights about the heteroatom doping into the carbon nanotubes could benefit the development of the carbon nanotube based functional materials and extend their application in a broad range of areas.

关键词： single-walled carbon nanotube (SWnT) array chemical vapor deposition (CVD) N-doping diameter dependent doping Raman spectroscopy

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Low-temperature nH_(3) abatement via selective oxidation over a supported copper catalyst with high Cu^(+) abundance

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Journal of Environmental Sciences 2024年第9期143卷 12-22页

作者： Zhiming Yang Lin Peng Leneng Yang Mingli Fu Daiqi Ye Peirong Chen Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control National Engineering Laboratory for VOCs Pollution Control Technology and EquipmentSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China Guangdong Chengyi Environmental Technology Corp. Shaoguan 512158China

Selective catalytic nH_(3)-to-n_(2) oxidation(nH_(3)-SCO)is highly promising for abating nH_(3) emissions slipped from stationary flue gas after-treatment devices.Its practical application,however,is limited by the non-availability of low-cost catalysts with high activity and n_(2) selectivity.Here,using defect-rich nitrogen-doped carbon nanotubes(nCnT-AW)as the support,we developed a highly active and durable copper-based nH_(3)-SCO catalyst with a high abundance of cuprous(Cu^(+))sites.The obtained Cu/nCnT-AW catalyst demonstrated outstanding activity with a T_(50)(i.***.the temperature to reach 50% nH_(3) conversion)of 174℃ in the nH_(3)-SCO reaction,which outperformed not only the Cu catalyst supported on n-free O-functionalized CnTs(OCnTs)or nCnT with less surface defects,but also those most active Cu catalysts in open literature.Reaction kinetics measurements and temperature-programmed surface reactions using nH_(3)as a probe molecule revealed that the nH_(3)-SCO reaction on Cu/nCnT-AW follows an internal selective catalytic reaction(i-SCR)route involving nitric oxide(nO)as a key intermediate.According to mechanistic investigations by X-ray photoelectron spectroscopy,Raman spectroscopy,and X-ray absorption spectroscopy,the superior nH_(3)-SCO performance of Cu/nCnT-AW originated from a synergy of surface defects and n-dopants.Specifically,surface defects promoted the anchoring of Cu O nanoparticles on n-containing sites and,thereby,enabled efficient electron transfer from n to Cu O,increasing significantly the fraction of SCR-active Cu^(+)sites in the catalyst.This study puts forward a new idea for manipulating and utilizing the interplay of defects and n-dopants on carbon surfaces to fabricate Cu^(+)-rich Cu catalysts for efficient abatement of slip nH_(3)emissions via selective oxidation.

关键词： nH_(3)-SCO XAnES Localized etching N-doping n_(2) selectivity i-SCR

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Dynamic photoelectrical regulation of ECM protein and cellular behaviors

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Bioactive Materials 2023年第4期22卷 168-179页

作者： Xiaozhao Wang Cai Yao Xudong Yao Junxin Lin Rui Li Kun Huang Weiming Lin Xiaojun Long Chao Dai Jiajun Dong Xuegong Yu a Wenwen Huang Wenjian Weng Qi Wang Hongwei Ouyang Kui Cheng School of Materials Science and Engineering State Key Laboratory of Silicon MaterialsCyrus Tang Center for Sensor Materials and ApplicationsZhejiang UniversityHangzhou310027China Dr.Li Dak Sum&Yip Yio Chin Center for Stem Cells and Regenerative Medicine Department of Orthopedic Surgery of the Second Affiliated HospitalZhejiang University School of MedicineHangzhou310058China Department of Sports Medicine Zhejiang University School of MedicineHangzhou310058China Zhejiang University-University of Edinburgh Institute Zhejiang University School of MedicineKey Laboratory of Tissue Engineering and Regenerative Medicine of Zhejiang ProvinceZhejiang University School of MedicineHangzhou314400China China Orthopedic Regenerative Medicine Group(CORMed) Hangzhou310058China School of Chemistry Zhejiang UniversityHangzhou310027China International Institutes of Medicine The Fourth Affiliated HospitalZhejiang University School of MedicineNo.N1Shangcheng AvenueYiwu322000China

Dynamic regulation of cell-extracellular matrix(ECM)-material interactions is crucial for various biomedical applications.In this study,a light-activated molecular switch for the modulation of cell attachment/detachment behaviors was established on monolayer graphene(Gr)/n-type Silicon substrates(Gr/Si).Initiated by light illumination at the Gr/Si interface,pre-adsorbed proteins(bovine serum albumin,ECM proteins collagen-1,and fibronectin)underwent protonation to achieve negative charge transfer to Gr films(N-doping)throughπ-πinteractions.This N-doping process stimulated the conformational switches of ECM proteins.The structural alterations in these ECM interactors significantly reduced the specificity of the cell surface receptor-ligand interaction(e.g.,integrin recognition),leading to dynamic regulation of cell adhesion and eventual cell detachment.RnA-sequencing results revealed that the detached bone marrow mesenchymal stromal cell sheets from the Gr/Si system manifested regulated immunoregulatory properties and enhanced osteogenic differentiation,implying their potential application in bone tissue regeneration.This work not only provides a fast and feasible method for controllable cells/cell sheets harvesting but also gives new insights into the understanding of cell-ECM-material communications.

关键词： Graphene Protein conformational change Charge transfer Cell-materials interaction N-doping

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Toward stable photoelectrochemical water splitting using niOOH coated hierarchical nitrogen-doped ZnO-Si nanowires photoanodes

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Journal of Energy Chemistry 2022年第8期31卷 45-55,I0002页

作者： Indrajit V.Bagal Maheswari Arunachalam Ameer Abdullah Aadil Waseem Mandar AKulkarni Soon Hyung Kang Sang-Wan Ryu Department of Physics Chonnam National UniversityGwangju 61186Republic of Korea Department of Chemistry Education Chonnam National UniversityGwangju 61186Republic of Korea Optoelectronic Convergence Research Center Chonnam National UniversityGwangju 61186Republic of Korea

Photoelectrochemical(PEC)water splitting is regarded as the most promising method to generate“green hydrogen”,and zinc oxide(ZnO)has been identified as one of the promising candidates for PEC water splitting owing to its straddling band alignment with the water redox level.However,its PEC performance is limited due to its wide bandgap and anticipated by photocorrosion in an aqueous medium.In this work,we present strategic improvements in the PEC water splitting performance of ZnO nanowires(nWs)by nitrogen(n)-doping along with photostability by the core–shell deposition of a niOOH cocatalyst.Highly crystalline hierarchical ZnO nWs were fabricated on Si nWs(ZnO-Si HnWs)using a metal organic chemical vapor deposition approach.The nWs were then n-doped by annealing in an nH_(3) atmosphere.The n-doped ZnO-Si HnWs(n:ZnO-Si HnWs)showed enhanced visible light absorption,and suppressed recombination of the photogenerated carriers.As compared to ZnO-Si HnWs(0.045 m A cm^(-2) at 1.23 V vs RHE),the n:ZnO-Si HnWs(0.34 m A cm^(-2) at 1.23 V vs RHE)annealed in nH^(3) ambient for 3 h at 600℃showed 7.5-fold enhancement in the photocurrent density.niOOH-deposited n:ZnO-Si HnW photoanodes with a photostability of 82.21%over 20000 s showed 10.69-fold higher photocurrent density(0.48 m A cm^(-2) at 1.23 V vs RHE)than ZnO-Si HnWs.

关键词： Hierarchical nWs MOCVD niOOH cocatalyst N-doping Photoelectrochemical water splitting

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