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Tailored heterostructured Ni_(3)N-NiO nano-frameworks for boosting electrocatalytic oxygen evolution via surface-modulated plasma strategy

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Nano Research 2024年第9期17卷 7909-7917页

作者： Bo Ouyang Haonan Qin Chao Sun Yilin Deng Ang Li Jipeng Zhu erjun kan Rajdeep Singh Rawat MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science&TechnologyNanjing 210094China The Laboratory of Road and Bridge Civil EngineeringSchool of ScienceNanjing University of Science&TechnologyNanjing 210094China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China Natural Sciences and Science Education National Institute of EducationNanyang Technological University637616Singapore

The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of H2 through heterostructure *** chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured ***,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction *** our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a Ni_(3)N-NiO heterostructure(hNiNO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hNiNO *** resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline *** stands in stark contrast to the performance of NiO-covered Ni_(3)N fabricated using the conventional plasma method(sNiNO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the Ni_(3)N-NiO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.

关键词： structural modulation auxiliary insulator-confined plasma surface heating control heterostructure electrocatalytic O2 evolution

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Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2) photoreduction via alternately hydrophobic surfaces

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Journal of Energy Chemistry 2024年第6期93卷 202-212,I0006页

作者： Hailing Huo Ting Hu Chengxi Huang Fang Wu Tongyu Wang Xuan Liu Liang Zhang Qiang Ju Zhiqing Zhong Hongbin Xing erjun kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion *** a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of ***,there is a contradiction in wettability requirements for the two ***,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)***,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic *** was achieved through a selectively hydrophobic modification method and a charge-transfer-control ***,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark *** innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： Hydrophobic Hydrophilic Gas transport Overall CO_(2)photoreduction Z-scheme

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High-density triple-phase contact points for enhanced photocatalytic CO_(2) reduction to methanol

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Chinese Chemical Letters 2024年第2期35卷 252-256页

作者： Hanwen Jian Kaiming Deng Tongyu Wang Chengxi Huang Fang Wu Hailing Huo Bo Ouyang Xuan Liu Jingjing Ma erjun kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science and TechnologyNanjing 210094China College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China

The efficiency of photocatalytic CO_(2) reduction reaction(PCRR)is restricted by the low solubility and mobility of CO_(2) in water,poor CO_(2) adsorption capacity of catalyst,and competition with hydrogen evolution reaction(HER).Recently,hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points(TPCPs)of CO_(2)(gas phase),H_(2) O(liquid phase),and catalysts(solid phase)near the surface of the catalyst,enabling direct delivery of highly concentrated CO_(2) molecules to the active reaction sites,resulting in higher CO_(2) and lower H+surface *** TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed ***,the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO_(2) adsorption ***,based on constructing a hydrophobic hierarchical porous TiO_(2)(o-HPT)with interconnected macropores and mesopores structure,we have significantly increased the density of TPCPs in a unit volume of the *** with hydrophobic macroporous TiO_(2)(o-MacPT)or mesoporous TiO_(2)(o-MesPT),the o-HPT with increased TPCP density leads to enhanced photoactivity,enabling a high methanol production rate with 1111.5μmol g^(−1) h^(−1) from *** results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.

关键词： Photocatalysis CO_(2)reduction reaction Photocatalyst Triple-phase contact points Methanol

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四面体超晶格中高温铁磁半导体的预测

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Science China Materials 2024年第4期67卷 1225-1230页

作者：王亚奇孙华胜吴世海李盎万逸阚二军黄呈熙 MIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 10094China

铁磁(FM)半导体兼具半导体(如逻辑器件)和磁性材料(如记忆存储器)的优点,半个多世纪以来一直受到广泛关注.然而,铁磁半导体的发展受到候选材料稀缺以及居里温度低的阻碍.铁磁性通常在具有八面体配位的过渡金属化合物中被发现.而具有较... 详细信息

铁磁(FM)半导体兼具半导体(如逻辑器件)和磁性材料(如记忆存储器)的优点,半个多世纪以来一直受到广泛关注.然而,铁磁半导体的发展受到候选材料稀缺以及居里温度低的阻碍.铁磁性通常在具有八面体配位的过渡金属化合物中被发现.而具有较小晶体场分裂和较弱反铁磁(AFM)直接交换的四面体配位化合物可能是高温铁磁体的潜在候选者,但很少被探索.在这项工作中,我们提出了高温铁磁半导体可以在四面体配位超晶格(SL)中实现.在第一性原理计算的基础上,我们系统地研究了一系列MX/TMX (MX表示12-16,13-15或14-14族四面体半导体,TM表示3d过渡金属,X表示配体)超晶格.其中,SiC/CrC SL是一种稳定的铁磁半导体材料,具有0.363 eV的间接带隙和~935 K的高居里温度.此外,我们还探讨了Cr原子层的分布和层间磁耦合,预测了单轴应变引起了反铁磁到铁磁的相变.这些发现为实现四面体配位超晶格的高温铁磁半导体在未来自旋电子应用中开辟了新的机会.

关键词：过渡金属化合物高居里温度自旋电子晶体场分裂超晶格逻辑器件八面体配位候选者

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Enhancing the activity of FeNi bimetallic electrocatalysts on overall water splitting by Nd_(2)O_(3)-induced FeNi lattice contraction

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Journal of Energy Chemistry 2023年第12期87卷 42-50,I0003页

作者： Jiajia Li Yunong Qin Tianyu Tan Qiancheng Zhu Bo Ouyang erjun kan Wenming Zhang Province-Ministry Co-construction Collaborative Innovation Center of Hebei Photovoltaic Technology College of Physics Science and TechnologyHebei UniversityBaoding 071002HebeiChina MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina

The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable ***,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal *** synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH ***,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice ***,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic ***,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.

关键词： Bifunctional catalyst FeNi-Nd_(2)O_(3)hetero-trimers Lattice contraction Overall water splitting

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Nitrogen doped porous carbon-based bifunctional oxygen electrocatalyst with controllable phosphorus content for zinc-air battery

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Nano Research 2023年第4期16卷 5887-5893页

作者： Shichang Cai Zihan Meng Gaojie Li Yu An Yapeng Cheng erjun kan Bo Ouyang Haining Zhang Haolin Tang School of Material Science and Engineering Henan University of TechnologyZhengzhou 450001China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong LaboratoryXianhu Hydrogen ValleyFoshan 528200China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Applied Physics and Institution of Energy and Microstructure Nanjing University of Science and TechnologyNanjing 210094China

The controllable construction of non-noble metal based bifunctional catalysts with high activities towards oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is of great significance,but remains a ***,we reported an effective method to synthesize cobalt-nitrogen doped mesoporous carbon-based bifunctional oxygen electrocatalyst with controllable phosphorus content(Co-N-P_(X)-MC,X=0.5,1.0,1.5,2.0).The mesoporous carbon substrate endowed the asprepared samples with more exposed active surface(236.50 m^(2)·g^(−1))and the most appropriate doping ratio of phosphorus had been investigated to be 1.5(Co-N-P1.5-MC).For ORR,Co-N-P1.5-MC exhibited excellent catalytic activity with more positive onset potential(1.01 V)and half-wave potential(0.84 V)than the other *** OER,Co-N-P1.5-MC also showed a low overpotential of 415 *** experimental results and density-functional theory(DFT)calculations,the outstanding bifunctional catalytic performance of Co-N-P1.5-MC was due to the synergistic cooperation between the P and N dopants,which could reduce the reaction barriers and was favorable for ORR and ***,the Zn-air battery using Co-N-P1.5-MC as the cathode showed remarkable battery performance with high stability(could operate stably for over 160 h at 10 mA·cm^(−2))and maximum power density(119 mW·cm^(−2)),demonstrating its potential for practical *** work could provide significant enlightenment towards the design and construction of bifunctional oxygen electrocatalyst for next-generation electrochemical devices.

关键词： cobalt-nitrogen doped porous carbon phosphorus doping bifunctional electrocatalyst oxygen reduction reaction(ORR)and oxygen evolution reaction(OER) Zn-air battery

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Room-temperature vertical ferroelectricity in rhenium diselenide induced by interlayer sliding

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Frontiers of physics 2023年第5期18卷 143-151页

作者： Fang Li Jun Fu Mingzhu Xue You Li Hualing Zeng erjun kan Ting Hu Yi Wan MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing and Department of Applied PhysicsNanjing University of Science and TechnologyNanjing 210094China International Center for Quantum Design of Functional Materials(ICQD) Hefei National Laboratory for Physical Sciences at the Microscaleand Department of PhysicsUniversity of Science and Technology of ChinaHefei 230026China State Key Laboratory for Artificial Microstructure&Mesoscopic Physics School of PhysicsPeking UniversityBeijing 100871China

One variety of ferroelectricity that results from lateral relative movements between the adjacent atomic layers is referred to as sliding ferroelectricity,which generates an interfacial charge transfer and hence a polarization *** mechanism of sliding ferroelectricity existent in van der Waals crystals is quite distinct from the conventional ferroelectric switching mechanisms mediated by ion *** creates new possibilities for the design of two-dimensional(2D)ferroelectrics since it can be achieved even in non-polar *** 2D ferroelectrics can be widely employed for practical implementations,however,there is still significant work to be done on several fronts,such as exploring ferroelectricity possibly in more potential 2D ***,we report the experimental observation of room-temperature robust vertical ferroelectricity in layered semiconducting rhenium diselenide(ReSe_(2)),a representative member of the transition metal dichalcogenides material family,based on a combined research of nanoscale piezoresponse and second harmonic generation *** no such ferroelectric behavior was seen in 1L ReSe_(2),2L ReSe_(2)exhibits vertical ferroelectricity at ambient *** on density-functional theory calculations,we deduce that the microscopic origin of ferroelectricity for ReSe_(2)is uncompensated vertical charge transfer that is dependent on in-plane translation and switchable upon interlayer *** findings have important ramifications for the ongoing development of sliding ferroelectricity since the semiconducting properties and low switching barrier of ReSe2 open up the fascinating potential for functional nanoelectronics applications.

关键词： rhenium diselenide transition metal dichalcogenides vertical ferroelectricity sliding ferroelectricity

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Nucleation of Boron-Nitrogen on Transition Metal Surface:A First-Principles Investigation

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Chinese Journal of Chemical Physics 2018年第3期31卷 335-340,368页

作者： Dildar Ahmed erjun kan Department of Applied Physics and Institution of Energy and MicrostructureNanjing University of Science and TechnologyNanjing 210094China

Boron nitrogen(BN)monolayer has attracted considerable attention because of their suc-cessful incorporation with graphene based ***,many important aspects of the growth mechanisms are still not well *** density functional theory(DFT)calculations,we found that Cu(111)surface is more suitable to be used as a substrate to grow BN monolayer compared with Ni(111)***,we explored that one-dimensional(1D)BN chain configuration is dominant to the two-dimensional(2D)BN ring formation from one pair to five BN pairs deposited on Cu(111)*** stable structure transformation of BN monolayer from 1D BN chain to 2D BN ring occurs when the number of pairs is n>*** is suggested that,as the number of BN pairs increases the energetically stable structures achieve.

关键词： Growth mechanism Density functional theory BN monolayer

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Enhanced charge separation by continuous homojunction with spatially separated redox sites for hydrogen evolution

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Nano Research 2023年第10期16卷 12323-12330页

作者： Mingyuan Yu Tongyu Wang Chengxi Huang Fang Wu Xuan Liu Hailing Huo Hanwen Jian Zikun Liang Jingjing Ma erjun kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science and TechnologyNanjing 210094China College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China

Photocatalytic hydrogen generation represents a promising strategy for the establishment of a sustainable and environmentally friendly energy ***,the current solar-to-hydrogen conversion efficiency is not yet sufficient for practical hydrogen production,highlighting the need for further research and ***,we report the synthesis of a Sn-doped TiO_(2)continuous homojunction hollow sphere,achieved through controlled calcination *** incorporation of a gradient doping profile has been demonstrated to generate a gradient in the band edge energy,facilitating carrier orientation ***,the hollow sphere’s outer and inner sides provide spatially separated reaction sites allowing for the separate acceptance of holes and electrons,which enables the rapid utilization of carriers after *** a result,the hollow sphere TiO_(2)with gradient Sn doping exhibits a significantly increased hydrogen production rate of 20.1 mmol·g^(−1)·h^(−1).This study offers a compelling and effective approach to the designing and fabricating highly efficient nanostructured photocatalysts for solar energy conversion applications.

关键词： continuous homojunction spatially separated reaction sites charge separation hydrogen evolution

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Nature of spin-lattice coupling in two-dimensional CrI3 and CrGeTe3

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Science China(Physics,Mechanics & Astronomy) 2021年第8期64卷 67-75页

作者： Jing Li JunSheng Feng PanShuo Wang erjun kan HongJun Xiang Key Laboratory of Computational Physical Sciences (Ministry of Education) State Key Laboratory of Surface Physicsand Department of Physics Fudan University Shanghai Qi Zhi Institute School of Physics and Materials Engineering Hefei Normal University Department of Applied Physics and Institution of Energy and Microstructure Nanjing University of Science and Technology Collaborative Innovation Center of Advanced Microstructures

Spin-lattice (SL) coupling plays an important role in spintronic applications given its effects on magnetic,ferroelectric,optical,and thermodynamic *** and theoretical calculations have revealed a large SL coupling effect in CrGeTe3and ***,the microscopic origin of SL coupling in these systems is still *** this work,we develop a systematic method to explore the atomistic mechanism of SL coupling based on the density functional *** find that the first-and second-order SL couplings in ternary system CrGeTe3are considerably stronger than those in binary system *** the first-order SL coupling,the Cr ions of the magnetic pair and Ge ions positively contribute to the strain enhancement of ferromagnetism in ***,the Cr ions provide a negative contribution in ***,our tight-binding analysis suggests that the p-d hopping in CrGeTe3gradually decreases with the tensile strain,rapidly enhancing the ferromagnetism under the tensile *** large frequency shifts in CrGeTe3are caused by the large second-order exchange derivatives (one type of second-order SL coupling) of the Cr ions of the magnetic pair.

关键词： spin-lattice effect two-dimensional magnetic materials first-principle calculation

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