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Introducing Spin Polarization into Mixed-Dimensional Van der Waals Heterostructures for High-Efficiency visible-light photocatalysis

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Energy & Environmental Materials 2023年第5期6卷 192-200页

作者： Yong Wang Wei Xu Yu Zhang Chengxin Zeng Weining Zhang Lin Fu Mei Sun Yizhang Wu Jian Hao Wei Zhong Youwei Du Rusen Yang Academy of Advanced Interdisciplinary Research School of Advanced Materials and NanotechnologyXidian UniversityXi'an 710126China National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures and Jiangsu Provincial Key Laboratory for NanotechnologyNanjing UniversityNanjing 210093China Department of Physics Shaanxi University of Science and TechnologyXi'an 710021China Department of Physics State Key Laboratory of Surface PhysicsFudan UniversityShanghai 200433China State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China

The low separation efficiency of the photogenerated carrier and the poor activity of the surface redox reaction are the main barrier to further improvement of photocatalytic materials.To address these issues,introducing spin-polarized electrons in single-component photocatalytic materials emerged as a promising approach.However,the decreased redox ability of photocarriers in these materials becomes a new challenge.Herein,we mitigate this challenge with a carbon nitride sheet(CNs)/graphene nanoribbon(GNR)composite material that has a van der Waals heterostructures(vdWHs)and spin-polarized electron properties.Experimental results and theoretical calculations show that the heterostructure has a strong redox ability,high carrier-separation efficiency,and enhanced surface catalytic reaction.Consequently,the mixed-dimensional CNs/GNR vdWHs exhibit remarkable performance for H_(2)and O_(2)generation as well as CO_(2)production under visible-light irradiation without any cocatalyst.The spin-polarized vdWHs discovered in this study revealed a new type of photocatalytic materials and advanced the development of spintronics and photocatalysis.

关键词： DFT calculations spin polarization Van der Waals heterostructures visible-light photocatalysis

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Metal-free synthesis of nitriles from aldehydes and ammonium by visible-light photocatalysis

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Science China Chemistry 2023年第10期66卷 2852-2857页

作者： Xu He Yi-Wen Zheng Bin Chen Ke Feng Chen-Ho Tung Li-Zhu Wu Key Laboratory of Photochemical Conversion and Optoelectronic Materials New Cornerstone Science LaboratoryTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Future Technology University of Chinese Academy of SciencesBeijing 100049China BayRay Innovation Center Shenzhen Bay LaboratoryShenzhen 518107China

A green method for synthesis of nitriles from aldehydes and ammonium salts under air is developed under extremely mild conditions,i.e.,1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4Cz IPN)as a photocatalyst,2,2,6,6-tetrametylpiperidine-1-oxyl(TEMPO)as a cocatalyst,and oxygen(ambient air)as the terminal oxidant,visible light irradiation of substrate solutions,producing the desired nitriles with excellent yields.The reaction involves two distinct transformations,imine formation between an aldehyde and an ammonium salt and photocatalytic oxidation of the formed imine by air to a nitrile.

关键词： visible-light photocatalysis aldehydes nitriles metal-free ambient air

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Constructing metal-free heterophotocatalyst using two-dimensional carbon nitride sheets and violet phosphorene for highly efficient visible-light photocatalysis

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Journal of Materials Science & Technology 2023年第15期146卷 113-120页

作者： Yong Wang Chengxin Zeng Liting Wu Yalin Dong Yu Zhang Dingyi Yang Wen Hu Jian Hao Hongzhe Pan Rusen Yang Academy of Advanced Interdisciplinary Research School of Advanced Materials and NanotechnologyXidian UniversityXi’an 710126China Department of Physics Shaanxi University of Science and TechnologyXi’an 710021China State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China School of Physics and Electronic Engineering Linyi UniversityLinyi 276005China

Two-dimensional(2D)carbon nitride sheets(CNs)with nanoscale thickness have great potential in solar energy conversion owing to their intrinsic bandgap.However,their photocatalytic efficiency falls far below the practical requirements because the generated electron-hole pairs rapidly recombine.We construct a metal-free 2D p–n junction heterophotocatalyst from CNs and violet phosphorene(VP)using a simple electrostatic self-assembly method.The experimental results and density functional theory calculations show that the built-in electric field of the p–n junction promotes photogenerated carrier transport at the heterojunction interface,thereby promoting the separation of photogenerated electron-hole pairs.Under visible-light illumination,the visible-light photocatalytic hydrogen and CO production rates of the CNs/VP heterojunction were increased by 5.85 and 1.51 times,respectively,when compared to that of CNs.This study provides new insights into the design of metal-free heterogeneous photocatalysts with high catalytic activity。

关键词： Heterostructures DFT calculations visible-light photocatalysis

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Novel Sc-doped Bi_(3)TiNbO_(9) ferroelectric nanofibers prepared by electrospinning for visible-light photocatalysis

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Journal of Rare Earths 2023年第3期41卷 365-373,I0002页

作者： Zhixiong Song Shuwen Yu Kaixian Wang Zhengming Jiang Liyan Xue Fan Yang Fujian Institute of Research on the Structure of Matter Chinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350002China Xiamen Institute of Rare Earth Materials Haixi InstituteChinese Academy of SciencesXiamen 361021China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Chinese Academy of SciencesXiamen 361021China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341001China

In this work,a novel Sc-doped Bi_(3)TiNbO_(9) ferroelectric nanofiber was first prepared by electrospinning.The nanofibers are approximately 100 nm level in diameter.The photocatalytic activity analysis reveals that the Bi_(3)TiNbO_(9) nanofibers synthesized by electrospinning are superior to powders prepared by the solid-state method,which is mainly attributed to the high specific surface area and high surface activity of the nanofibers.In addition,doping Sc can reduce the band gap of Bi_(3)TiNbO_(9) and further improve the photocatalytic efficiency.Bi_(3)TiNbO_(9) nanofibers containing 5 mol%Sc have the highest photocatalytic activity,which can degrade 98.55%of RhB under 405 nm light irradiation for 120 min.In addition,the catalytic mechanism of the catalyst was obtained by scavenger tests,active species capture tests and band structure analyses.After three cycles of photocatalytic experiment,the degradation rate is decreased by only 2.42%,proving that the nanofibers catalyst has excellent stability.This work provides good prospects for the practical application of electrospinning technology in the field of photocatalysis.

关键词： Nanofibers Ferroelectric Scandium visible-light photocatalysis Rare earths

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Plasma-exfoliated g-C_(3)N_(4) with oxygen doping: tailoring photocatalytic properties

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Frontiers of Chemical Science and Engineering 2024年第2期18卷 27-39页

作者： Yuxin Li Junxin Guo Rui Han Zhao Wang National Engineering Research Centre of Industry Crystallization Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Heteroatom doping and defect engineering have been proposed as effective ways to modulate the energy band structure and improve the photocatalytic activity of g-C_(3)N_(4). In this work, ultrathin defective g-C_(3)N_(4) was successfully prepared using cold plasma. Plasma exfoliation reduces the thickness of g-C_(3)N_(4) from 10 nm to 3 nm, while simultaneously introducing a large number of nitrogen defects and oxygen atoms into g-C_(3)N_(4). The amount of doped O was regulated by varying the time and power of the plasma treatment. Due to N vacancies, O atoms formed strong bonds with C atoms, resulting in O doping in g-C_(3)N_(4). The mechanism of plasma treatment involves oxygen etching and gas expansion. Photocatalytic experiments demonstrated that appropriate amount of O doping improved the photocatalytic degradation of rhodamine B compared with pure g-C_(3)N_(4). The introduction of O optimized the energy band structure and photoelectric properties of g-C_(3)N_(4). Active species trapping experiments revealed ·O_(2)^(–) as the main active species during the degradation.

关键词： graphitic carbon nitride cold plasma oxygen doping nitrogen defect visible-light photocatalysis

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Facile synthesis of hierarchical NiO/NiFe2O4 microsphere composite as efficient visible photocatalyst for 2,4-DCP degradation

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Rare Metals 2024年第4期43卷 1580-1588页

作者： Shabana Shaheen Shuai Xu Ji Bian Amir Zada Zi-Qing Zhang Yang Qu Li-Qiang Jing Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education) International Joint Research Center and Lab for Catalytic TechnologySchool of Chemistry and Materials ScienceHeilongjiang University Department of Chemistry Abdul Wali Khan University

It is highly desired to develop efficient photocatalysts with recycling property for practical application to degrade toxic pollutants.Herein,nanosheet-assembled NiFe2O4microspheres with commendable activity are successfully synthesized by a facile solvothermal reaction with NH4F as the modifier,and their photoactivities are further improved by coupling with NiO through an in situ growth process.The optimized nickel oxide（NiO）/nickel ferrite（NiFe2O4） microsphere composite（5NiO/NFO-4）exhibits a satisfactory photocatalytic activity for 2,4-dichlorophenol（2,4-DCP） degradation under visible-light irradiation,which is attributed to its wide visible-light response,well-designed hierarchical structure and enhanced charge transfer and separation by coupling NiO as a high-level energy platform to accept electrons.Moreover,it is found that the NiO/NiFe2O4microsphere photocatalysts can be easily collected and recycled owing to the distinctive magnetic properties.This work provides a feasible route to rational design visible-light-driven photocatalysts with high-activity for environmental remediation and purification with good recyclability.

关键词： NiFe 2 O 4 microspheres NiO/NiFe 2 O 4 composite Charge separation visible-light photocatalysis 2,4-Dichlorophenol degradation

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Enhanced visible-light photocatalytic hydrogen evolution using two-dimensional carbon nitride sheets with the removal of amine groups

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Chinese Chemical Letters 2024年第2期35卷 446-450页

作者： Yu Zhang Liting Wu Shaopeng Wang Dingyi Yang Huan Liang Yizhang Wu Jian Hao Youqing Wang Jianke Liu Yong Wang Department of Physics Shaanxi University of Science and TechnologyXi'an 710021China School of Advanced Materials and Nanotechnology Academy of Advanced Interdisciplinary ResearchXidian UniversityXi'an 710126China The State Key Discipline Laboratory of Wide Band Gap Semiconductor Technology Xidian UniversityXi'an 710126China Collaborative Innovation Center of Advanced Microstructures National Laboratory of Solid State MicrostructuresNanjing UniversityNanjing 210093China State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China

Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups,the practical applicability of CNs in photocatalysis is limited.In this study,CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing.The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV,increasing their absorption of visible light.Interestingly,the CNs were distorted after annealing,which can differentiate the spatial positions of electrons and holes,enhancing the visible-light absorption efficiency.As a result,when exposed to visible light,the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times.This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.

关键词： 2D carbon nitride sheets Rapid thermal annealing DFT calculations visible-light absorption visible-light photocatalysis

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Continuous microflow visible-light photocatalytic N-formylation of piperidine and its kinetic study

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Chinese Chemical Letters 2024年第1期35卷 285-289页

作者： Yangyang Xu Fang Zhao Xuhong Guo State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China International Joint Research Center of Green Energy Chemical Engineering Shanghai 200237China

N-formylation of amines,a class of synthetically important reactions,is typically conducted using metal catalysts that are relatively expensive or not readily available and usually needs harsh conditions to increase the reaction efficiency.Here,an efficient continuous microflow strategy was developed for the gas-liquid visible-light photocatalytic N-formylation of piperidine,which achieved a reaction yield of 82.97%and a selectivity of>99%at 12 min using cheap organic dye photocatalyst under mild reaction conditions.The influence of essential parameters,including light intensity,temperature and equivalents of the gas,additive and photocatalyst,on the reaction yield was systematically studied.Furthermore,kinetic investigations were conducted,exhibiting the dependence of reaction rate and equilibrium yield of N-formylpiperidine on light intensity,temperature and photocatalyst equivalent.The microflow photocatalytic approach established in this work,which realized a markedly higher space-time yield than the conventional batch method(37.9 vs.0.212 mmol h-1 L-1),paves the way for the continuous,green and efficient synthesis of N-formamides.

关键词： Microflow visible-light photocatalysis N-Formylation Piperidine Kinetics

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Anti-Markovnikov ring-opening of sulfonium salts with alkynes by visible light/copper catalysis

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Science China Chemistry 2023年第3期66卷 791-798页

作者： Xuan Li Min Jiang Junze Zuo Xiuyan Song Jian Lv Daoshan Yang Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science Ministry Of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 310036China Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China

Internal alkynes are widespread skeletons in bioactive molecules and materials which are also used as important building blocks in chemical synthesis. Herein, we report a novel and efficient copper-catalyzed Sonogashira reaction between sulfonium salts and alkynes through an anti-Markovnikov ring-opening pathway promoted by visible light. The coexistence of the nitrogen and phosphorus ligands in the system is the key to the success of this reaction. This radical type ring-opening reaction affords a new strategy for the synthesis of internal alkynes. Furthermore, this study is also an effective complement to the diverse reaction patterns of sulfonium salts.

关键词： radical reaction visible-light photocatalysis sulfonium salts copper catalysis alkynes

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A 3D/0D cobalt-embedded nitrogen-doped porous carbon/supramolecular porphyrin magnetic-separation photocatalyst with highly efficient pollutant degradation and water oxidation performance

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Journal of Materials Science & Technology 2022年第29期124卷 53-64页

作者： Lufang Ning Jing Xu Yang Lou Chengsi Pan Zhouping Wang Yongfa Zhu State Key Laboratory of Food Science and Technology Jiangnan UniversityWuxi 214122China School of Food Science and Technology Jiangnan UniversityWuxi 214122China International Joint Laboratory on Food Safety Jiangnan UniversityWuxi 214122China Collaborative Innovation Center of Food Safety and Quality Control in Jiangsu Province Jiangnan UniversityWuxi 214122China Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China National Engineering Research Center for Functional Food Jiangnan UniversityWuxi 214122China Key Laboratory of Meat Processing of Sichuan Chengdu UniversityChengdu 610106China Department of Chemistry Tsinghua UniversityBeijing 100084China

A 3D/0D cobalt-embedded nitrogen-doped porous carbon nanocubes(Co-N-C)/supramolecular tetra(4-carboxylphenyl)porphyrin nanocrystals(SA-TCPP)photocatalyst was successfully self-assembled viaπ–πinteraction,hydrogen bonding,and chemical bonding.Co-N-C/SA-TCPP heterostructure exhibited satisfactory visible photocatalytic oxidation performance on pollutant degradation and water evolution.The degradation rates of Co-N-C/ST(30%)composite towards 2,4-dichlorophenol,ofloxacin,and ethylene were10.9,7.2,and 2.1 times faster than SA-TCPP,respectively.The oxygen evolution efficiency was 1.9 times higher than SA-TCPP.The remarkably improved oxidation activities of Co-N-C/SA-TCPP were mainly ascribed to the following reasons:(1)Co-N-C could enhance the light absorption ability of SA-TCPP to produce more photoinduced carriers.(2)The well-developed porosity of Co-N-C could optimize the dispersibility of SA-TCPP to provide more reactive sites and charge separation channels.(3)Theπ–πinteraction between SA-TCPP and Co-N-C was beneficial to interlayer charge mobility,while the embedded cobalt nanoparticles(Co NPs)and N-doped carbon matrix could serve as electron traps to accelerate interfacial electron transfer.Additionally,the ferromagnetic Co NPs endowed Co-N-C/SA-TCPP with magnetic-separation function to promote recyclability in practical application.

关键词： visible-light photocatalysis Supramolecular porphyrin ZIF-67 derived co-catalyst 3D/0D heterostructure Magnetic-separation

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