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One-step supramolecular preorganization constructed crinkly graphitic carbon nitride nanosheets with enhanced photocatalytic activity

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Journal of Materials Science & Technology 2022年第9期104卷 155-162页

作者： Songcan Wang Yuelin Li Xin Wang Guohao Zi Chenyang Zhou Boyan Liu Gang Liu Lianzhou Wang Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical University127 West Youyi RoadXi’an 710072China Honors College Northwestern Polytechnical University127 West Youyi RoadXi’an 710072China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandQLD 4072Australia Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences72 Wenhua RoadShenyang 110016China School of Materials Science and Engineering University of Science and Technology of China72 Wenhua RoadShenyang 110016China

Here we report a new one-step thermal polycondensation process to form crinkly graphitic carbon nitride nanosheets(CGCNNs)via supramolecular preorganization,using a mixture of urea and melamine as the starting *** studies reveal that the newly developed CGCNNs significantly strengthen the optical absorption,widen the bandgap,and increase the Hall mobility and carrier density compared to that of its bulk counterpart,regardless of the similar chemical composition and *** a result,the photocatalytic hydrogen production rate is improved by 7 ***,Na doping of CGCNNs can further promote its photocatalytic activity,leading to an excellent photocatalytic hydrogen production rate of 250.9μmol h^(–1),which is approximately 10.5 times higher than its bulk ***,an impressive apparent quantum efficiency of 19.12%is achieved at 420 *** study provides a facile strategy for the design of efficient low-cost carbon-nitride-based photocatalysts for solar fuel production.

关键词： carbon nitride Supramolecular preorganization Hall mobility Na doping Solar hydrogen

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Hierarchical Self-assembly of Well-Defined Louver-Like P-Doped carbon nitride Nanowire Arrays with Highly Effcient Hydrogen Evolution

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Nano-Micro Letters 2020年第4期12卷 76-91页

作者： Bo Li Yuan Si Qian Fang Ying Shi Wei‑Qing Huang Wangyu Hu Anlian Pan Xiaoxing Fan Gui‑Fang Huang Department of Applied Physics College of Physics and Electronicsand College of Materials Science and Engineeringand State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082People’s Republic of China Department of Physics and Tsinghua‑Foxconn Nanotechnology Research Center Tsinghua UniversityBeijing 100084People’s Republic of China College of Physics Liaoning UniversityShenyang 110036People’s Republic of China

Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced ***,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent ***,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen *** this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity ***,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high ***,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 *** experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and *** findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.

关键词： Self-assembly carbon nitride P-doped Nanowire arrays Hydrogen evolution

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New carbon nitride close to C_(6)N_(7) with superior visible light absorption for highly efficient photocatalysis

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Science Bulletin 2021年第17期66卷 1764-1772,M0004页

作者： Xinyu Zhao Yingnan Zhao Huaqiao Tan Huiying Sun Xing Qin Wingkei Ho Min Zhou Jinliang Lin Yangguang Li Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal UniversityChangchun 130024China Department of Science and Environmental Studies The Education University of Hong KongHong KongChina

The rational design and construction of novel two-dimensional(2D)carbon nitrides(CNs)beyond g-C_(3)N_(4) is a hot topic in the fields of chemistry and *** by the polymerisation of urea,we have prepared a series of novel C-C bridged heptazine CNs UO_(x)(where x is the ratio of urea to oxamide,x=1,1.5,2,2.5,and 3),which are similar to(C_(6)N_(7))n,upon the introduction of *** predicted using density functional theory(DFT)calculations,the conjugated structure of UO_(x) was effectively extended from an individual heptazine to the entire ***,its bandgap was reduced to 2.05 eV,and its absorption band edge was significantly extended to 600 ***,its carrier transfer and separation were significantly enhanced,establishing its superior photocatalytic *** optimised UO_(2) exhibits a superior photocatalytic hydrogen production rate about 108.59 lmol h^(-1)(using 10 mg of catalyst)with an apparent quantum efficiency(AQE)of 36.12%and 0.33%at 420 and 600 nm,respectively,which is one of the most active novel CNs reported to ***,UO_(2) exhibits excellent photocatalytic activity toward the oxidation of diphenylhydrazine to azobenzene with conversion and selectivity reaching~100%,which represents a promising highly efficient 2D CN *** phenols degradation,UO_(2) also displayed significantly higher activity and durability during the degradation of phenol when compared to traditional g-C_(3)N_(4),highlighting its significant potential for application in energy,environment and photocatalytic organic reactions.

关键词： carbon nitride Urea Oxamide Photocatalytic hydrogen production Photocatalytic oxidation of diphenylhydrazine

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State-of-the-art progress in overall water splitting of carbon nitride based photocatalysts

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Frontiers in Energy 2021年第3期15卷 600-620页

作者： Bing LUO Yuxin ZHAO Dengwei JING School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China International Research Center for Renewable Energy and State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049China

Converting solar energy into hydrogen(H_(2))by photocatalytic water splitting is a promising approach to simultaneously address the increasing energy demand and environmental *** decade has passed since the discovery of photo-induced water splitting phenomenon on TiO_(2)photoanode,while the solar to H_(2) efficiency is still around 1%,far below the least industrial ***,developing efficient photocatalyst with a high energy conversion efficiency is still one of the main tasks to be *** carbon nitride(g-C_(3)N_(4))is just such an emerging and potential ***,in this review,the state-of-the-art advances in g-C_(3)N_(4)based photocatalysts for overall water splitting were summarized in three sections according to the strategies used,and future challenges and new directions were discussed.

关键词： photocatalysis overall water splitting carbon nitride hydrogen

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A unique and well-designed 2D graphitic carbon nitride with sponge-like architecture for enhanced visible-light photocatalytic activity

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Journal of Materials Science & Technology 2023年第28期159卷 99-111页

作者： Mahdieh Razi Asrami Milad Jourshabani Min Hee Park Daiha Shin Byeong-Kyu Lee Department of Civil and Environment Engineering University of UlsanDaehakro 93NamguUlsan 680-749Republic of Korea Western Seoul Center Korea Basic Science InstituteSeoul 03759Republic of Korea

A unique and well-designed 2D graphitic carbon nitride(g-CN)with sponge-like architecture has been successfully synthesized by engineering supramolecular self-assembly and well-organized SiO 2 *** resulting material showed great optical and textural characteristics with plenty of open and uni-form pores,which are very helpful whether for multiple light scattering or mass *** formation of boosted delocalizedπ-conjugated electrons at the molecular level and condensed heptazine building blocks result in enhanced carrier density and charge transfer *** emission spectroscopy and time-resolved fluorescence lifetime(TRPL)strongly confirmed the enhancement of light harvesting and prolonged charge carrier *** optimized sample exhibited a degradation performance of 95%of bisphenol A(BPA,10 mg L-1)after 60 min under visible-light irradiation at pH=*** the scavenging experiments,probing experiments as well as electron paramagnetic resonance(EPR)confirm that•O 2-is the dominant reactive species that fragments bisphenol ***,density functional theory(DFT)calculations unveil that the BPA interaction with a modified g-CN containing porous structure is energeti-cally more favorable than non-porous pure ***,the toxicity assessment showed that the final degradation products were placed in the non-harmful category based on acute and chronic *** study presents a promising strategy to modify the g-CN properties and provides an efficient technique for boosting its visible-light photocatalytic activity.

关键词： Sponge-like carbon nitride Photocatalysis Visible-light

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Structure and Tribology Property of carbon nitride Films Deposited by MW-ECR Plasma Enhanced Unbalanced Magnetron Sputtering

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Plasma Science and Technology 2006年第4期8卷 425-428页

作者：高鹏徐军朴勇丁万昱邓新绿董闯 State Key Laboratory of Materials Modification by Laser Ion and Electron BeamsDalian University of TechnologyDalian 116024China State Key Laboratory of Materials Modification by Laser Ion and Electron BeamsDalian University of TechnologyDalian 116024China International Centre for Materials PhysicsChinese Academy of SciencesShenyang 110016China

carbon nitride films were deposited by a twinned microwave electron cyclotron resonance （ECR） plasma source enhanced unbalanced magnetron sputtering system. The results indicate that the structure of the films is sensitive to the nitrogen content. The increase in the nitrogen flow ratio leads to an increase in the sp3 content and an improvement of the tribological properties.

关键词： carbon nitride tribological property unbalanced magnetron sputtering

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Synthesis of band gap-tunable alkali metal modified graphitic carbon nitride with outstanding photocatalytic H_2O_2 production ability via molten salt method

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Journal of Materials Science & Technology 2018年第10期34卷 1932-1938页

作者： Xiaoyu Qu Shaozheng Hu Jin Bai Ping Li Guang Lu Xiaoxue Kang Liaoning Key Laboratory of Petroleum & Chemical Industry Liaoning Shihua University Fushun 113001 China

Band gap-tunable alkali metal modified graphitic carbon nitride was prepared by a molten salt method. X-ray diffraction, N2 isothermal sorption, ultraviolet-visible spectroscopy, scanning electron microscope, X-ray photoelectron spectroscopy and photoluminescence were used to characterize the obtained cat-alysts. The photocatalytic H202 production ability of as-prepared catalyst was investigated. The results indicate that K＋ and Na＊ are doped into g-CBN4 lattice simultaneously by the molten salt method. Alkali metal modification not only promotes the specific surface area, visible light absorption and separation of electron-hole pairs, but tunes the conduction band and valence band edge positions of as-prepared catalysts by controlling the weight ratio of eutectic salts to melamine. The tunable band edge positions result in the photocatalytic H202 production from ＂single channel pathway＂ to ＂two channel pathway＂, leading to the promoted H202 production ability.

关键词： Molten salt carbon nitride Banding structure Visible light photocatalyst Photocatalysis

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Cobalt atoms dispersed on hierarchical carbon nitride support as the cathode electrocatalyst for high-performance lithium-polysulfide batteries

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Science Bulletin 2019年第24期64卷 1875-1880页

作者： Jialing Wu Junmei Chen Yang Huang Kun Feng Jun Deng Wei Huang Yunling Wu Jun Zhong Yanguang Li Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Soochow University

Lithium-sulfur batteries are promising candidates for next-generation energy storage but are confronted with several challenges. One of the possible solutions is to design proper cathode electrocatalysts to accelerate the redox interconversion of solvated polysulfide intermediates. Herein, we report cobalt atoms dispersed on hierarchical carbon nitride support as an effective cathode electrocatalyst for lithium-polysulfide batteries. The electrocatalyst material is prepared from the simple reaction between melamine and cyanuric acid in the presence of Co^2+, followed by the Ar annealing. The product has a unique hierarchical structure consisting of many thin and porous C3 N4 nanosheets finely dispersed with Co atoms. The atomic dispersion of Co species is confirmed by X-ray absorption *** measurements reveal that it can promote the interconversion of polysulfides. As a result,batteries using this cathode electrocatalyst achieve large capacity($1400 mAh/g at 1.6 mA/cm^2), good rate performance($800 mAh/g at 12.8 mA/cm^2) and impressive cycling stability under different current densities and different sulfur loadings.

关键词： Li-polysulfide battery Cathode electrocatalyst carbon nitride Cobalt single atom

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One-pot synthesis of array-like sulfur-doped carbon nitride with covalently crosslinked ultrathin MoS cocatalyst for drastically enhanced photocatalytic hydrogen evolution

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Journal of Materials Science & Technology 2021年第16期75卷 59-67页

作者： Shumin Zhang Hu Dong Changsheng An Zhongfu Li Difa Xu Kaiqiang Xu Zhaohui Wu Jie Shen Xiaohua Chen Shiying Zhang College of Materials Science and Engineering Hunan UniversityChangsha410082China Hunan Key Laboratory of Applied Environmental Photocatalysis Changsha UniversityChangsha 410005Hunan ProvinceChina School of Physics and Electronics Hunan Normal University410081China

Constructing noble-metal-free loaded catalyst with high-efficiency photocatalytic activity by a simple and scalable method is of profound significance for fundamental research and practical ***,a simple one-pot method was used to synthesize novel samples of array-like sulfur-doped graphitic carbon nitride(SCN)nanosheets with ultrathin MoS2 loading(MS/SCN-x%).The ultrathin MoS2 cocatalyst was evenly distributed on the surface of SCN and was linked to the main catalyst by covalent chemical *** from the multiple advantages of the array-like porous nanosheets structure with rich exposed surface,covalent cross-linking structure,and enhanced visible light absorption,the MS/SCN-2.5%composites drastically improve hydrogen evolution performance,which is superior to original MoS2 nanosheet modified by two-step mixing method,and also rivals with Pt/*** designing strategy of photocatalyst modified by noble-metal-free cocatalyst with covalent bond structure provides fascinating insights into enhanced photocatalytic hydrogen evolution.

关键词： carbon nitride Noble-metal-free cocatalyst Covalent cross-linking Photocatalytic hydrogen evolution

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Influence of Bias on the Properties of carbon nitride Films Prepared by Vacuum Cathodic Arc Method

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Journal of Materials Science & Technology 2004年第6期20卷 735-738页

作者： Zhimin ZHOU, Lifang XIA and Mingren SUNSchool of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China Sch. of Mat. Sci. and Eng. Harbin Inst. of Technol. Harbin 150001 China

carbon nitride films have been synthesized in a wide range of biases from 0 to -900 V by vacuum cathodic arc method. The N content was about 12.0-22.0 at. pct. Upon increasing the biases from 0 to -100 V, the N content increased from 15.0 to 22.0 at. pct which could be attributed to the knot-on effect. While the further increasing biases led to the gradual falling of the N content to 12.0 at. pct at -900 V due to the enhancement of the sputtering effect. Below -200 V, with the increasing biases the sp2C fraction in the films decreased, as a result of vvhich the I(D)/I(G) fell in the Raman spectra and the sp peaks also showed the decreasing tendency relative to the s peaks in the VBXPS (valence band X-ray photoelectron spectroscopy). While above -200 V, the sp2C fraction increased and the films became graphitinized gradually, accompanying which the I(D)/I(G) rose from -200 V to -300 V and the Raman spectra even shovved the graphite characteristic above -300 V and the sp peaks rose again relative to the s peak. The carbon nitride films mainly consist of three types of bonding: CC, sp2CN and sp3CN bonds. In the first stage the sp3CN relative ratio rises and falls in the second stage, which corresponded well with the variation of the sp2C in the films. The subpiantation mechanism resulting from the effect of ion energy played an important role in deciding'the variation of the microstructure of the carbon nitride films.

关键词： carbon nitride Vacuum cathodic arc Raman spectroscopy X-ray photoelectron spectroscopy

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