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Doping transition metal in PdSeO_(3)atomic layers by aqueous cation exchange:A new doping protocol for a new 2D photocatalyst

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Chinese Chemical Letters 2022年第8期33卷 3739-3744页

作者： Xiuming Zhang Rongrong Pan Tailei Hou Shuping Zhang Xiaodong Wan Yuemei Li Shan Liu Jia Liu Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

Elemental doping confined in atomically-thin 2 D semiconductors offers a compelling strategy for constructing high performance *** impressive progress has been achieved based on co-thermolysis method,the choices of dopants as well as semiconductor hosts are still quite limited to yield the elaborate photocatalyst with atomic-layer-confined doping defects,owing to the difficulty in balancing the reaction kinetics of different *** study shows that the cation exchange reaction,which is dictated by the Pearson's hard and soft acids and bases(HSAB)theory and allowed to proceed at mild temperatures,can be developed into a conceptually new protocol for engineering elemental doping confined in semiconductor atomic *** this aim,the two atomic layers of a new type of 2 D photocatalyst PdSe0_(3)(PdSe0_(3)2 ALs,1.1 nm)are created by liquid exfoliation and exploited as a proof-of-concept *** is demonstrated that the Mn(Ⅱ)dopants with controlled concentrations can be incorporated into PdSeO_(3)2 ALs via topological Mn^(2+) for-Pd^(2+) cation exchange performed in water/isopropanol solution at 30℃.The resulting Mn-doped PdSeO_(3)2 ALs present enhanced capacity for driving photocatalytic oxidation reactions in comparison with their undoped *** findings here suggest that the new route mediated by post synthetic cation exchange promises to give access to manifold 2 D confined-doping photocatalysts,with little perturbations on the thickness,morphology,and crystal structure of the atomically-thin semiconductor hosts.

关键词： 2D Semiconductor Atomic layers Photocatalysis Doping Cation exchange

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Size-effect on Ni electrocatalyst:The case of electrochemical benzyl alcohol oxidation

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Nano Research 2023年第1期16卷 202-208页

作者： Jian Zhong Yongli Shen Pei Zhu Shuang Yao Changhua An Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion School of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China Tianjin Key Laboratory of Advanced Functional Porous Materials Institute for New Energy Materials&Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

The nanoparticles(NPs)of Ni with different sizes endows its distinctive physical and chemical properties,which represents a typical strategy for the development of high-performance ***,the size effect of metallic Ni-NPs on electrocatalytic performance remains ***,the Ni-NPs with different sizes supported on nitrogen doped carbon(NC)has been synthesized by controlling the pyrolysis temperature,leading to the synthesis of Ni@NC-500(8.3 nm),Ni@NC-280(1.9 nm)and Ni@NC-200(1.0 nm).The electrooxidation of benzyl alcohol(BA)over these nanocatalysts shows the yield of benzoic acid was 99%,82%,55%on Ni@NC-280,Ni@NC-200 and Ni@NC-500,*** experimental and theoretical simulation demonstrate that the difference in the adsorption strength of reactant molecules by Ni-NPs is responsible for their different performance,where the Ni@NC-280 exhibits an optimal adsorption configuration between Ni@NC-280 electrode and *** work provides a new angle for designing and synthesizing efficient electrocatalysts,which may be extended to the exploration of various promising electrocatalytic systems.

关键词： size effect electro-oxidation Ni nanoparticles benzyl alcohol

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Atomically dispersed dual Fe centers on nitrogen-doped bamboo-like carbon nanotubes for efficient oxygen reduction

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Nano Research 2022年第3期15卷 1966-1972页

作者： Ligang Ma Junlin Li Zhiwei Zhang Hao Yang Xueqin Mu Xiangyao Gu Huihui Jin Ding Chen Senlin Yan Suli Liu Shichun Mu School of Electronic Engineering Nanjing Xiaozhuang UniversityNanjing 211171China Nanjing Key Laboratory of Optometric Materials and Technology Jinling Institute of TechnologyNanjing 211169China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Key Laboratory of Advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China

Interfacial atomic configuration between dual-metal active species and nitrogen-carbon substrates is of great importance for improving the intrinsic activity of catalysts toward oxygen reduction reaction(ORR).Thus,from the atomic-scale engineering we develop a high intrinsic activity ORR catalyst in terms of incorporating atomically dispersed dual Fe centers(single Fe atoms and ultra-small Fe atomic clusters)into bamboo-like N-doped carbon *** from atomically dispersed dual-Fe centers on the atomic interface of Fe-Nx/carbon nanotubes,the fabricated dual Fe centers catalyst exhibits an extremely high ORR activity(E_(onset)=1.006 V;E_(1/2)=0.90 V),beyond state-of-the-art Pt/***,this catalyst also shows a superior kinetic current density of 19.690 mA·cm^(−2),which is 7 times that of state-of-the-art Pt/***,based on the excellent catalyst,the primary Zn-air battery reveals a high power density up to 137 mW·cm^(−2) and sufficient potential cycling stability(at least 25 h).Undoubtedly,given the unique structure–activity relationship of dual-Fe active species and metal-nitrogen-carbon substrates,the catalyst will show great prospects in highly efficient electrochemical energy conversion devices.

关键词： atomic configuration single Fe atoms atomically dispersed Fe clusters N-doped bamboo-like carbon nanotubes oxygen reduction reaction

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Layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals for enhanced photocatalytic CO_(2) reduction

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Nano Research 2022年第7期15卷 5953-5961页

作者： Shuang Zhao Qian Liang Zhongyu Li Hong Shi Zhenyu Wu Hui Huang Zhenhui Kang Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Institute of Functional Nano and Soft Materials Laboratory(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering Macao University of Science and TechnologyTaipa 999078MacaoChina Institute of Advanced Materials Northeast Normal UniversityChangchun 130024China

Halide perovskite nanocrystals are potential catalysts for CO_(2) photoreduction,while,the strong radiative recombination and insufficient stability limit their catalytic performance and ***,we report that layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals(CLDH)for enhanced photocatalytic CO_(2) *** CLDH heterojunctions show the remarkably enhanced CO_(2) photoreduction performance;without cocatalyst and sacrificial agent,the average electron consumption rate of CLDH(49.16μmol·g^(−1)·h^(−1))is approximately 3.7 times higher than that of pristine CsPbBr_(3).Also,CLDH catalyst exhibits a robust stability after ten cycles over 30 h.

关键词： CsPbBr_(3) NiAl-LDH CO_(2)reduction Z-scheme photocatalysis

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Metalphthalocyanine frameworks grown on TiO_(2)nanotubes for synergistically and efficiently electrocatalyzing urea production from CO_(2)and nitrate

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science China Chemistry 2023年第5期66卷 1417-1424页

作者： Ning Li Hui Gao Zhixin Liu Qianjun Zhi Bowen Li Lei Gong Baotong Chen Tao Yang Kang Wang Peng Jin Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China Innovation Research Institute for Carbon Neutrality University of Science and Technology BeijingBeijing 100083China

Electrocatalytic synthesis of urea from CO_(2)and NO_(3)^(-)under ambient conditions provides an appealing alternative to the traditional energy-intensive urea synthetic *** active and selective electrocatalysts for efficient urea production are therefore urgently desired owing to the unsatisfactory performance of the thus far reported ***,a phthalocyaninebased(Pc-based)covalent organic framework(COF),namely Co Pc-COF,fabricated from the nucleophilic substitution reaction of hexadecafluorophthalocyaninato cobalt with octahydroxylphthalocyanine cobalt,in situ grew on the surface of multilayered Ti O_(2)nanotubes(NTs),generating the Co Pc-COF@Ti O_(2)NTs *** X-ray diffraction analysis in combination with electron microscopy measurements discloses the uniform coating of crystalline Co Pc-COF on the multilayered Ti O_(2)NTs in Co Pc-COF@Ti O_(2)***,electrochemical tests reveal the superior electrocatalytic activity of Co Pc-COF@Ti O_(2)NTs towards urea production from CO_(2)and NO3-with a record-high yield of 1,205μg h^(-1)cm^(-2)and an outstanding Faraday efficiency of 49%at-0.6 V versus reversible hydrogen electrode due to the significant synergistic catalysis *** situ attenuated total reflection infrared spectroscopic investigation and theoretical calculations unveil the efficient C–N coupling reaction between*CO intermediate derived from CO_(2)on Co Pc moieties and*NH2intermediate formed from NO_(3)^(-)on Ti O_(2)NTs during the urea formation process over Co Pc-COF@Ti O_(2)*** work should be helpful towards designing and fabricating high-performance electrocatalysts for sustainable synthesis of urea through efficient synergistic effect of multiactive centers.

关键词： covalent organic frameworks phthalocyanine TiO_(2) electrocatalytic urea synthesis C–N bond coupling

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Strong and conductive reduced graphene oxide-MXene porous films for efficient electromagnetic interference shielding

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Nano Research 2022年第6期15卷 4916-4924页

作者： Yu Zhang Ming-Ke Xu Zhenguo Wang Tianyu Zhao Liu-Xin Liu Hao-Bin Zhang Zhong-Zhen Yu State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China

Lightweight,flexible,and electrically conductive porous films are promising for efficient electromagnetic interference(EMI)***,the mechanical and electrical properties of porous films are far from ***,we fabricate mechanically flexible and electrically conductive reduced graphene oxide(rGO)-Ti_(3)C_(2)T_(x)MXene(rG-M)porous films with optimized continuous cellular morphology by a controlled hydrazine foaming *** presence of MXene prevents excessive expansion of the rG-M film,improves the electron conduction paths,and enhances the mechanical *** resultant rG-M porous film has superior mechanical and electric performances compared to its rGO counterpart,giving one of the highest tensile strengths(24.5 MPa)among the porous films,a high electrical conductivity of 74.4 S·cm^(−1),and an excellent broadband EMI shielding from 8 to 26.5 GHz.A high EMI shielding effectiveness of 52.6 dB is achieved for the porous film by adjusting its thickness and treatment procedure,providing a feasible fabrication route for lightweight and high-performance EMI shielding materials.

关键词： graphene MXene electromagnetic interference shielding porous films electrical conductivity

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Unexpected giant negative area compressibility in palladium diselenide

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National science Review 2023年第9期10卷 146-153页

作者： Xingxing Jiang Shengzi Zhang Dequan Jiang Yonggang Wang Maxim S.Molokeev Naizheng Wang Youquan Liu Xingyu Zhang Zheshuai Lin New Functional Crystals Group Key Laboratory of Functional Crystals and Laser TechnologyTechnical Institute of Physics and ChemistryChinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences University of Chinese Academy of Sciences Center for High Pressure Science &Technology Advanced Research School of Materials Science and Engineering Peking University Laboratory of Crystal Physics Kirensky Institute of PhysicsSB RAS Department of Physics Far Eastern State Transport University International Research Center of Spectroscopy and Quantum Chemistry Siberian Federal University

Negative area compressibility（NAC） is a counterintuitive 'squeeze-expand' behavior in solids that is very rare but attractive due to possible pressure-response applications and coupling with rich physicochemical ***,NAC behavior is reported in palladium diselenide with a large magnitude and wide pressure *** discover that,apart from the rigid flattening of layers that has been generally recognized,the unexpected giant NAC effect in PdSe2largely comes from anomalous elongation of intralayer chemical *** structural variations are driven by intralayer-to-interlayer charge transfer with enhanced interlayer interactions under *** work updates the mechanical understanding of this anomaly and establishes a new guideline to explore novel compression-induced properties.

关键词： negative area compressibility Lifshitz mechanism charge transfer

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Graphene oxide as a hole extraction layer loaded on BiVO_(4)photoanode for highly efficient photoelectrochemical water splitting

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Rare Metals 2022年第11期41卷 3795-3802页

作者： Min-Li Guo Shi-Peng Wan Cao-Long Li Kan Zhang Key Laboratory of Biomedical Functional Materials School of ScienceChina Pharmaceutical UniversityNanjing211198China Institute of Optoelectronics and Nanomaterials MIIT Key Laboratory of Advanced Display Material and DevicesCollege of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing210094China

The tailor-made oxygen evolution catalysts(OECs)paired with photoanodes offer a path to promote water oxidation kinetics;however,the unsatisfied interface between OECs and photoanode sets a barrier for efficient charge ***,a graphene oxide(GO)layer to promote the charge transfer from BiVO_(4)(BVO)to NiOOH OEC is *** is found that GO layer inserted between BVO and NiOOH can not only serve as hole extraction layer due to its hole storage capability,but also improve the ***,the rationally designed NiOOH/GO/BVO photoanode achieves a photocurrent density of 3.81 mA·cm^(-2)at 1.23 V(*** hydrogen electrode(RHE)),which is 3.85 times as high as that of bare *** work opens up low-cost auxiliary materials for enhancing photoelectrochemical water splitting.

关键词： BiVO_(4) Water splitting Charge extraction Oxygen evolution catalyst Graphene oxide

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Time-dependent color-tunable room temperature phosphorescence from unusual conformational transitions in phenothiazine polymers under UV irradiation

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science China Chemistry 2025年第3期68卷 1091-1098页

作者： Jiwen Lu Yifan Niu Chanjuan Jin Chengheng Wu Hanyu Wang Yan Guan Ping Wang Xinghe Fan Key Lab of Environment-Friendly Chemistry and Application of Ministry of Education Key Laboratory of Polymeric Materials and Application Technology of Hunan ProvinceKey Laboratory of Advanced Functional Polymer Materials of CollegesUniversities of Hunan ProvinceCollege of ChemistryXiangtan UniversityXiangtan 411105China Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Achieving color-tunable room-temperature phosphorescence(RTP),especially including blue RTP from a single-component polymer still faces a formidable ***,we wisely choose conformation-dependent phenothiazine with trifluoromethyl substituent as the side group of the phosphor monomer(Cz PT)and then copolymerize it with N-isopropylacrylamide(NIPAM)through photopolymerization to obtain polymers PPCz ***-dependent color-tunable phosphorescence from unusual quasi-equatorial(eq)to quasi-axial(ax)conformers are obtained,and the RTP color changes from orange(550 nm)to blue(470 nm)with phosphorescence lifetime up to 0.96 *** theoretical calculations confirm that the quasi-axial conformer is the preferred structure that facilitates the formation of intramolecular hydrogen bonds on the trifluoromethyl *** EPR spectra illustrate that the persistent UV irradiation generates radical cations to induce the conformational transitions first,followed by photopolymerization immobilizing the ax conformation in PPCz *** of data encryption and anti-counterfeiting are fabricated to show prompt and delayed multicolor *** work affords a simple and feasible avenue for two-dimensional color tunable room temperature phosphorescence from a single-component polymer.

关键词： polymeric room temperature phosphorescence color-tunable phosphorescence conformation-dependent time-dependent blue phosphorescence

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3D-printed Lunar regolith simulant-based geopolymer composites with bio-inspired sandwich architectures

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Journal of advanced Ceramics 2023年第3期12卷 510-525页

作者： Siqi Ma Yuqi Jiang Shuai Fu Peigang He Chengyue Sun Xiaoming Duan Dechang Jia Paolo Colombo Yu Zhou Institute for Advanced Ceramics School of Materials Science and EngineeringHarbin Institute of TechnologyHarbin 150001China Key Laboratory of Advanced Structural–Functional Integration Materials&Green Manufacturing Technology Harbin Institute of TechnologyHarbin 150001China Max Planck Institute for Polymer Research Mainz 5512Germany Laboratory for Space Environment and Physical Sciences Harbin Institute of TechnologyHarbin 150001China Department of Industrial Engineering University of PadovaPadova 35122Italy Department of Materials Science and Engineering The Pennsylvania State UniversityPhiladelphia 16802USA

Over time,natural materials have evolved to be lightweight,high-strength,tough,and damage-tolerant due to their unique biological ***,combining biological inspiration and structural design would provide traditional materials with a broader range of performance and ***,the application of an ink-based three-dimensional(3D)printing strategy to the structural design of a Lunar regolith simulant-based geopolymer(HIT-LRS-1 GP)was first reported,and high-precision carbon fiber/quartz sand-reinforced biomimetic patterns inspired by the cellular sandwich structure of plant stems were *** study demonstrated how different cellular sandwich structures can balance the structure–property relationship and how to achieve unprecedented damage tolerance for a geopolymer *** results presented that components based on these biomimetic architectures exhibited stable non-catastrophic fracture characteristics regardless of the compression direction,and each structure possessed effective damage tolerance and anisotropy of mechanical *** results showed that the compressive strengths of honeycomb sandwich patterns,triangular sandwich patterns,wave sandwich patterns,and rectangular sandwich patterns in the Y-axis(Z-axis)direction were 15.6,17.9,11.3,and 20.1 MPa(46.7,26.5,23.8,and 34.4 MPa),respectively,and the maximum fracture strain corresponding to the above four structures could reach 10.2%,6.7%,5.8%,and 5.9%(12.1%,13.7%,13.6%,and 13.9%),respectively.

关键词： Lunar regolith simulant(LRS) three-dimensional(3D)printing geopolymer(GP) in situ resource utilization(ISRU) bio-inspired patterns damage tolerance

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