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Covalent triazine frameworks modified by ultrafine Pt nanoparticles for efficient photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 4908-4915页

作者： Xu Han Xueying Ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma school of chemistry and Life science Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China Department of chemistry University of North Texas1508 W.Mulberry St.DentonTX 76201USA Department of chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia

Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen *** this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active *** fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine *** calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production ***,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic *** overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.

关键词： Pt nanoparticles covalent triazine-based framework-1(CTF-1) photocatalysts hydrogen evolution reaction

Unraveling the role of NiSnPH@OOH/CC perovskite hydroxide for efficient electrocatalytic oxidation of methanol to formate

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Nano Research 2024年第4期17卷 2388-2399页

作者： Jing Shao Yusheng Fang Xiaobing Wu Muhammad Imran Abdullah Youkun Tao college of chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China school of science Harbin Institute of TechnologyShenzhen 518055China

The sluggish kinetics of oxygen evolution reaction(OER)is the key tailback for hydrogen production from the water *** OER with thermodynamically auspicious methanol oxidation reaction(MOR)can significantly boost the H_(2) and value-added products ***,it is currently challenging to achieve a synergistic manipulation of product selectivity and performance for MOR ***,we report NiSnPH@OOH/CC(CC=carbon cloth)perovskite hydroxide nanosphere as an efficient MOR electrocatalyst with high activity,stability,and selectivity towards methanol oxidation to formate.A surface amorphous layer of defect rich NiOOH was generated in operando by selective Sn leaching with stable perovskite hydroxide bulk structure,which mitigates the oxidative power and optimizes the local coordination environment of the active NiOOH *** situ Raman combined with electrochemical studies further confirm the key active species,NiOOH,generated in operando enhance the MOR and blocking the over oxidation of methanol to CO_(2).As a result,NiSnPH@OOH/CC effectively masks the OER and attains>99%selectivity with 100%Faradic efficiency for *** results of this study show the advances of NiSnPH@OOH/CC as an efficient electrocatalyst for MOR and also suggest its potential applications for various small organic molecules oxidation.

关键词： perovskite hydroxide small organic molecules nickel oxy(hydroxide) value-added products methanol oxidation reaction

Conductive catalysis by subsurface transition metals

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National science Review 2024年第1期11卷 86-93页

作者： Xin Deng Caiyan Zheng Yangsheng Li Zeyu Zhou Jiamin Wang Yihua Ran Zhenpeng Hu Fan Yang Landong Li Frontiers science Center for New Organic Matter College of ChemistryNankai University school of Physics Nankai University school of Physical science and Technology Shanghai Tech University school of Materials science and Engineering Nankai University Haihe Laboratory of Sustainable Chemical Transformations

The nature of catalysis has been hotly pursued for over a century, and current research is focused on understanding active centers and their electronic structures. Herein, the concept of conductive catalysis is proposed and verified by theoretical simulations and experimental observations. Metallic systems containing buried catalytically active transitional metals and exposed catalytically inert main group metals are constructed, and the electronic interaction between them via metallic bonding is disclosed. Through the electronic interaction, the catalytic properties of subsurface transitional metals(Pd or Rh) can be transferred to outermost main group metals(Al or Mg) for several important transformations like semi-hydrogenation,Suzuki-coupling and hydroformylation. The catalytic force is conductive, in analogy with the magnetic force and electrostatic force. The traditional definition of active centers is challenged by the concept of conductive catalysis and the electronic nature of catalysis is more easily understood. It might provide new opportunities for shielding traditional active centers against poisoning or leaching and allow for precise regulation of their catalytic properties by the conductive layer.

关键词： electronic interaction conductive catalysis subsurface transition metal

Mechanism research progress on transition metal compound electrode materials for supercapacitors

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Rare Metals 2024年第9期43卷 4076-4098页

作者： Zhi-Hui Xu Xue-Lei Li Qing-Wen Li Kai Lv Jing-Shun Liu Xiu-Kun Hang Aruuhan Bayaguud school of Materials science and Engineering Inner Mongolia University of Technology school of Materials science and Engineering Tianjin University of Technology college of chemistry and Chemical Engineering Inner Mongolia University

Supercapacitors(SCs) have remarkable energy storage capabilities and have garnered considerable interest due to their superior power densities and ultra-long cycling characteristics. However, their comparatively low energy density limits their extensive application in large-scale commercial applications. Electrode materials directly affect the performance of SCs. Thus, the development of cutting-edge electrode materials and modification of their morphological and structural properties are vital for advancing the performance of SCs. Transition metal compounds have a high specific capacity and good cycling durability, making them the most promising electrode active materials for high-energy density SCs. Nevertheless,their inadequate conductivity, unfavorable ion diffusion rates, substantial volume expansion and phase transitions during charging and discharging are obstacles to their stable and efficient integration into SCs. To address these challenges, this study provides a comprehensive summary of the current advancements in transition metal nanomaterials as electrode materials for SCs, an overview of the current research status, and the prevailing ***, this study highlights synthetic techniques and management strategies for electrode materials derived from transition metal compounds, targeting the resolution of the aforementioned challenges. Finally, a concise discussion is provided on the future directions of SC development, with an emphasis on the utilization of transition metal compound electrode materials.

关键词： Electrodes

Approaching the theoretical capacity of TiO_(2) anode in a photorechargeable lithium-ion battery

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Nano Research 2024年第4期17卷 2655-2662页

作者： Wen Yan Jie Wang Qing Hu Jingjing Fu Mohamed K.Albolkany Tian Zhang Xiao Lu Fei Ye Bo Liu school of chemistry and Materials science University of Science and Technology of ChinaHefei 230026China

New generation of lithium-ion batteries(LIBs)integrating solar energy conversion and storage is emerging,as they could solve the fluctuation problem in the utilization of solar ***-rechargeable lithium-ion batteries(PR-LIBs)are ideal devices for such target,in which solar energy is converted into electricity and stored in *** order to achieve the high performance of PR-LIB,it is crucial to develop dual-function electrode materials that can synergistically capture solar energy and store ***,we present photo-rechargeable lithium-ion batteries using defective black TiO_(2) as photoanode prepared by lithium *** photoanode exhibits excellent photo response in full solar spectrum with a capacity enhancement of 46.4%under illumination,corresponding to the energy conversion efficiency of 4.4%at the current density of 1 A·g^(-1).When illumination is applied at 20 mA·g^(-1),the battery capacity increases from~230 in dark to~349 mAh·g^(-1) at the first cycle,and then stabilizes at 310 mAh·g^(-1),approaching the theoretical value of 335 mAh·g^(-1) of TiO_(2) electrode *** finding provides thoughts for breaking the capacity limitations in TiO_(2) and paves the way for powering LIBs by solar illumination.

关键词： photo-rechargeable lithium-ion batteries photoanode defective TiO_(2)(D-TiO_(2))

Topological Structure-Modulated Collagen Carbon as Two-in-One Energy Storage Configuration toward Ultrahigh Power and Energy Density

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Energy & Environmental Materials 2024年第2期7卷 22-33页

作者： Li Yuan Wenlong Cai Yunhong Wei Yiran Pu Can Liu Yun Zhang Hao Wu college of Materials science and Engineering Sichuan University Department of Applied chemistry University of Science and Technology of China

Efficient energy storage devices with suitable electrode materials,that integrate high power and high energy,are the crucial requisites of the renewable power source,which have unwrapped new possibilities in the sustainable development of energy and the ***,a facile collagen microstructure modulation strategy is proposed to construct a nitrogen/oxygen dual-doped hierarchically porous carbon fiber with ultrahigh specific surface area(2788 m2g-1) and large pore volume(4.56 cm3g-1) via local microfibrous breakage/disassembly of natural structured *** operando spectroscopy and density functional theory unveil that the dual-heteroatom doping could effectively regulate the electronic structure of carbon atom framework with enhanced electric conductivity and electronegativity as well as decreased diffusion resistance in favor of rapid pseudocapacitive-dominated Li+-storage(353 mAh g-1at 10 A g-1).Theoretical calculations reveal that the tailored micro-/mesoporous structures favor the rapid charge transfer and ion storage,synergistically realizing high capacity and superior rate performance for NPCF-H cathode(75.0 mAh g-1at 30 A g-1).The assembled device with NPCF-H as both anode and cathode achieves extremely high energy density(200 Wh kg-1)with maximum power density(42 600 W kg-1) and ultralong lifespan（80%capacity retention over 10 000 cycles）.

关键词： collagen carbon energy storage device theoretical calculations topological structure modulation ultrahigh power and energy density

Towards wafer-scale growth of two-dimensional cerium dioxide single crystal with high dielectric performance

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Nano Research 2024年第9期17卷 8592-8599页

作者： Zhuofeng Shi Muhammad Imran Xiaohui Chen Xin Liu Yaqi Zhu Zhaoning Hu Saiyu Bu Jialin Zhang Chunhu Li Xiaodong Zhang Li Lin college of chemistry and Chemical Engineering Qingdao UniversityQingdao 266000China school of Materials science and Engineering Peking UniversityBeijing 100871China Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Key Laboratory of Marine chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

Owing to the atomically thin nature,two-dimensional(2D)oxide materials have been widely reported to exhibit exciting transport and dielectric properties,such as fine gate controllability and ultrahigh carrier mobility,that outperform their bulk ***,unlike the successful synthesis of bulk oxide single crystals,reliable methods for synthesizing large-area single crystal of 2D oxide,that would suppress the negative influence from defective grain boundaries,remain unavailable,especially for nonlayered ***,we report that the lattice symmetry between the substrate and cerium dioxide(CeO_(2))would allow for the aligned nucleation and epitaxial growth of CeO_(2)on sapphire substrates,enabling the wafer-sized growth of CeO_(2)single *** careful tuning of the growth temperature and oxygen flow rate contributed to the harvesting of CeO_(2)wafer with reduced thickness and enhanced growth *** removal of grain boundaries improved the dielectric performance in terms of high dielectric strength(E_(bd)≈8.8 MV·cm^(-1)),suppressed leakage current,along with high dielectric constants(ε_(r)≈24).Our work demonstrates that with fine dielectric performance and ease of synthesizing wafer-sized single crystals,CeO_(2)can function as potential candidate as gate insulator for 2D-materials based nanoelectronics,and we believe the reported protocol of aligned nucleation can be extended to other 2D oxides.

关键词： dielectric materials two-dimensional materials chemical vapor deposition cerium dioxide

Diatomic Fe-Co catalysts synergistically catalyze oxygen evolution reaction

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Nano Research 2024年第5期17卷 3794-3800页

作者： Tianmi Tang Jingyi Han Zhenlu Wang Xiaodi Niu Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China college of Food science and Engineering Jilin UniversityChangchun 130062China

The design of diatomic catalysts with uniformly dispersed metal atoms is expected to improve catalytic performance,which is conducive to the intensive comprehending of the synergistic mechanism between dual-metal sites for the oxygen evolution reaction(OER)at the atomic ***,we design a strategy to immobilize bimetallic Fe-Co atoms onto nitrogen-doped graphene to obtain a diatomic catalyst(DA-FC-NG)with FeN_(3)-CoN_(3) *** DA-FC-NG shows excellent OER activity with a low overpotential(η_(10)=268 mV),which is superior to commercial iridium dioxide *** calculations uncover that the excellent activity of DA-FC-NG is due to the interaction between Fe and Co diatoms,which causes charge rearrangement and induces the adsorption of intermediates on the Fe-O-Co bridge structure,thus improving the catalytic OER *** work is of great significance for the design of highly active diatomic catalysts to replace noble metal catalysts for energy-related applications.

关键词： oxygen evolution reaction diatomic catalyst FeN_(3)-CoN_(3) X-ray absorption spectroscopy(XAS)spectrum theoretical calculation

Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

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Rare Metals 2024年第4期43卷 1570-1579页

作者： Gang Dong Cong Huang Fei-Yang Chen Xue-Qin Liu Zhen Li Xiao-Li Su Tao Zeng Yun-Xia Chen Yi-Huang Chen Yang Wang school of Materials science and Engineering Jingdezhen Ceramic UniversityJingdezhen333403China Faculty of Materials science and chemistry China University of GeosciencesWuhan430074China college of chemistry and Materials Engineering Wenzhou UniversityWenzhou325035China

Given the clean and inexhaustible solar energy from solar light,photocatalytic ammonia synthesis is extremely ***,high electron-hole recombination rates and insufficient active sites severely limited N2 photoreaction ***,we designed and fabricated FeCu alloy nanoparticles anchored on carbon nitride nanosheets with excellent photocatalyt ic ammonia synthesis *** a coupler between Fe and carbon nitride,Cu promotes the separation of photogenerated charge carriers in carbon nitride under solar light irradiation,and renters the semiconductor a forceful electron donor for the Fe active *** accumulated electrons at Fe sites furtherly facilitated the adsorption and activation of the molecular ***,the uniform dispersed FeCu alloy nanoparticles were on carbon nitride nanosheets enhanced the stability of photocataly tic nitrogen reduction reaction,making the artificial photocataly tic ammonia synthesis more sustainable for *** work highlights that a direct electron transfer channel can be used to regulate the photochemical nitrogen fixation network.

关键词： Photocatalytic N_2 fixation Carbon nitride FeCu alloy Active sites Hydrogenation pathway

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