检索结果-南通市图书馆

Smart Interfacing between Co-Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High-efficiency electrocatalytic nitrogen reduction

在线全文

学校读者我要写书评

暂无评论

Energy & Environmental Materials 2023年第2期6卷 62-69页

作者： Xiaohui Wu Lu Tang Yang Si Chunlan Ma Peng Zhang Jianyong Yu Yitao Liu Bin Ding Key Laboratory of High Performance Fibers&Products(Ministry of Education) College of TextilesDonghua UniversityShanghai 201620China Innovation Center for Textile Science and Technology Donghua UniversityShanghai 200051China Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application School of Physical Science and TechnologySuzhou University of Science and TechnologySuzhou 215009China State Center for International Cooperation on Designer Low-carbon&Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China

Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.

关键词： density functional theory electrocatalytic nitrogen reduction graphitic carbon nitride interface engineering layered double hydroxide

Mesoporous MnO_(2)nanosheets for efficient electrocatalytic nitrogen reduction via high spin polarization induced by oxygen vacancy

在线全文

学校读者我要写书评

暂无评论

Nano Research 2023年第4期16卷 4664-4670页

作者： Yangyang Wen Jiahao Liu Feiran Zhang Zhenxing Li Ping Wang Zhao Fang Miao He Jingshuai Chen Weiyu Song Rui Si Lianzhou Wang State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum(Beijing)Beijing 102249China College of Science China University of Petroleum(Beijing)Beijing 102249China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandBrisbaneQLD 4072Australia

The electrochemical N_(2)reduction reaction(NRR)represents a green and sustainable route for NH_(3)synthesis under ambient conditions.However,the mechanism of N_(2)activation in the electrocatalytic NRR remains unclear.Herein,we found that the high spin state Mn^(3+)-Mn^(3+)pairs induced by oxygen vacancy in MnO_(2)nanosheets greatly enhance the catalytic activities.The strong electron transfer between d orbital of Mn and orbital of N2 forces the N_(2)to be of radical nature,which activates the hydrogenation process and weakens the N≡N bond.Based on the density functional theory(DFT)calculation results,we precisely designed mesoporous MnO_(2)nanosheets with rich oxygen vacancies via using methyltriphenylphosphonium bromide(MPB)to induce more Mn^(3+)-Mn^(3+)pairs(Mn^(3-3)-MnO_(2)),which can achieve a fairly high ammonia yield of up to 147.2μg·h^(−1)·mgcat−1.at−0.75 V vs.reversible hydrogen electrode(RHE)and a high Faradaic efficiency(FE)of 11%.Furthermore,these mesoporous MnO_(2)nanosheets exhibit the superior durability with negligible changes in both NH3 yield and FE after a consecutive 6-recycle test and the current density electrolyzed over a 24-hour period.Our findings offer an approach to designing highly active transition metal catalysts for electrocatalytic nitrogen reduction.

关键词： Mn^(3+)-Mn^(3+)pair MnO_(2)nanosheets mesopores ammonia synthesis electrocatalytic nitrogen reduction

Microfluidic platform serves as controllable fabrication of binary Mo/Ir nanodots/carbon hetero-material for efficient electrocatalytic nitrogen reduction

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Particuology 2023年第8期79卷 1-9页

作者： Hengyuan Liu Xingjiang Wu Jianhong Xu The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

electrocatalytic nitrogen reduction reaction(NRR)is regarded as a potential routine to achieve environment-friendly ammonia production,because of its abundant nitrogen resources,clean energy utilization and flexible operation.However,it is hindered by low activity and selectivity,in which con-dition well-designed catalysts are urgently in need.In this work,a binary Mo/Ir nanodots/carbon(Mo/Ir/C)hetero-material is efficiently constructed via microfluidic strategy,of which the nanodots are ho-mogeneously distributed on the carbon skeleton and the average size is approximately 1 nm.Excellent performance for NRR is obtained in 1 mol L^(-1) KOH,of which the optimized ammonia yield and faradic efficiency are 7.27μg h^(-1) cm^(-2) and 2.31%respectively.Moreover,the optimized ammonia yield of 6.20μg h-1 cm-2 and faradic efficiency of 10.59%are also obtained in 0.005 mol L^(-1) H_(2)SO_(4).This work achieves the continuous-flow synthesis and controllable adjustment of hetero-materials for favorable morphologies,which provides an innovative pathway for catalyst design and further promotes the development of ammonia production field.

关键词： Binary Mo/Ir nanodots Microfluidic platform Controllable fabrication Flexible modification electrocatalytic nitrogen reduction

Carbon Fiber Supported Binary Metal Sulfide Catalysts with Multi-Dimensional Structures for electrocatalytic nitrogen reduction Reactions Over a Wide pH Range

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Advanced Fiber Materials 2021年第4期3卷 229-238页

作者： Tianyi Zhang Wei Zong Yue Ouyang Yue Wu Yue-E Miao Tianxi Liu State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringInnovation Center for Textile Science and TechnologyDonghua University2999 North Renmin RoadShanghai 201620People’s Republic of China Research Center for Analysis and Measurement Donghua UniversityShanghai 201620People’s Republic of China Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122People’s Republic of China

Green and environmentally friendly electrocatalytic nitrogen(N_(2))fixation to synthesize ammonia(NH3)is recognized as an effective method to replace the traditional Haber-Bosch process.However,the difficulties in N_(2) adsorption and fracture of hard N≡N bond still remain major challenges in electrocatalytic N_(2) reduction reactions(NRR).From the perspectives of enhancing N_(2) adsorption and providing more catalytic sites,two-dimensional(2D)FeS_(2) nanosheets and three-dimensional(3D)metal organic framework-derived ZnS embedded within N-doped carbon polyhedras are grown on the carbon cloth(CC)template in this work.Thus,a composite NRR catalyst with multi-dimensional structures,which is signed as FeS_(2)/ZnS-NC@CC,is obtained for using over a wide pH range.The uniform distribution of hollow ZnS-NC frameworks and FeS_(2) nanosheets on the surface of CC largely increase the N_(2) enrichment efficiency and offer more active sites,while the CC skeleton acts as an independent conductive substrate and S-doping helps promote the fracture of N≡N bond during the NRR reaction.As a result,the FeS_(2)/ZnS-NC@CC electrode achieves a high Faraday efficiency of 46.84%and NH3 yield of 58.52μg h^(−1) mg^(−1) at-0.5 V vs.Ag/AgCl in 0.1 M KOH.Furthermore,the FeS_(2)/ZnS-NC@CC electrode displays excellent NRR catalytic activity in acidic and neutral electrolytes as well,which outperforms most previously reported electrocatalysts including noble metals.Therefore,this work provides a new way for the design of multi-dimensional electrocatalysts with excellent electrocatalytic efficiency and stability for NRR applications.

关键词： Multi-dimensional structure Heteroatom doping Carbon fiber cloth electrocatalytic nitrogen reduction

The pitfalls in electrocatalytic nitrogen reduction for ammonia synthesis

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Journal of Energy Chemistry 2021年第10期30卷 149-154,I0005页

作者： Huimin Liu Néstor Guijarro Jingshan Luo Institute of Photoelectronic Thin Film Devices and Technology Solar Energy Research CenterKey Laboratory of Photoelectronic Thin Film Devices and Technology of TianjinMinistry of Education Engineering Research Center of Thin Film Photoelectronic TechnologyRenewable Energy Conversion and Storage CenterNankai UniversityTianjin 300350China Institute of Electrochemistry University of AlicanteAlicante E-03080Spain

Ammonia synthesis by electrocatalytic nitrogen reduction reaction(EC-NRR)has gained momentum in recent years fueled by its potential to operate at ambient conditions,unlike the highly energyintensive yet long-standing Haber-Bosch process.However,the large disparity of the yields and Faradic efficiencies reported for EC-NRR raises serious concerns about the reliability of the experimental results.In this perspective,we elaborate on the potential sources of error when assessing EC-NRR and update the testing protocols to circumvent them,and more importantly,we pose a general call for consensus on ammonia production analysis and reporting to lay the solid foundations that this burgeoning field requires to thrive.

关键词： electrocatalytic nitrogen reduction Ammonia synthesis Pitfalls Standard protocols

FeNi@CNS nanocomposite as an efficient electrochemical catalyst for N_(2)-to-NH_(3) conversion under ambient conditions

在线全文

学校读者我要写书评

暂无评论

Journal of Materials Science & Technology 2022年第8期103卷 59-66页

作者： Tayiba Ilyas Fazal Raziq Nasir Ilyas Liuxin Yang Sharafat Ali Amir Zada Syedul Hasnain Bakhtiar Yong Wang Huahai Shen Liang Qiao School of Physics University of Electronic Science and Technology of ChinaChengdu 610054China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 10084China Department of Chemistry Abdul Wali Khan University of MardanMardanKPK 23200Pakistan Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Institute of Nuclear Physics and Chemistry Chinese Academy of Engineering PhysicsMianyang 621900China

The electrocatalytic nitrogen reduction reaction(NRR)has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia(NH_(3))synthesis.However,finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen(N_(2))for electrocatalytic NRR is still a challenge.Herein,a FeNi@CNS nanocomposite as an efficient catalyst for N_(2) fixation under ambient conditions is designed.This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination.The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst,which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83%and an NH_(3) yield of 16.52μg h^(−1) cm^(−2) in 0.1 M Na_(2)SO_(4) aqueous solution.Besides,high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h.Meanwhile,the FeNi@CNS catalyst encourages N_(2) adsorption and activation as well as effectively suppressing competitive HER.Therefore,this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.

关键词： electrocatalytic nitrogen reduction Transition-metal alloy FeNi@CNS catalyst N_(2)fixation to NH_(3)

Sulfur-deficient Bi_(2)S_(3-x) synergistically coupling Ti_(3)C_(2)T_(x)-MXene for boosting electrocatalytic N_(2) reduction

在线全文

学校读者我要写书评

暂无评论

Nano Research 2022年第5期15卷 3991-3999页

作者： Yaojing Luo Peng Shen Xingchuan Li Yali Guo Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

electrocatalytic nitrogen reduction reaction(NRR)is an appealing route for the sustainable NH_(3)synthesis,while developing efficientand durable NRR catalysts remains at the heart of achieving high-efficiency N_(2)-to-NH_(3)electrocatalysis.Herein,we rationally combine vacancy and interface engineering to design sulfur-deficient Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene as an effective NRR catalyst.The developed Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene(Bi2S3-xTi_(3)C_(2)T_(x))naturally contained abundant S-vacancies and exhibited a dramatically boosted NRR activity with an NH_(3)yield of 68.3μg·h^(-1)mg^(-1)(-0.6 V)and a Faradaic efficiency of 22.5%(-0.4 V),far superior to pure Bi_(2)S_(3)and Ti_(3)C_(2)T_(x)and surpassing almost all ever reported Bi-and MXene-based NRR catalysts.Theoretical investigations unveiled that the exceptional NRR activity of Bi_(2)S_(3-x)/Ti_(3)C_(2)T_(x)stemmed from its dual-active-center system involving both S-vacancies and interfacial-Bi sites,which could synergistically promote N_(2)adsorption and*N_(2)H formation to result in an energetic-favorable NRR process.

关键词： electrocatalytic nitrogen reduction bismuth catalyst MXene vacancy engineering interface engineering

Accelerated Discovery of Single-Atom Catalysts for nitrogen Fixation via Machine Learning

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Energy & Environmental Materials 2023年第1期6卷 377-383页

作者： Sheng Zhang Shuaihua Lu Peng Zhang Jianxiong Tian Li Shi Chongyi Ling Qionghua Zhou Jinlan Wang School of Physics Southeast UniversityNanjing 211189China

Developing high-performance catalysts using traditional trial-and-error methods is generally time consuming and inefficient.Here,by combining machine learning techniques and first-principle calculations,we are able to discover novel graphene-supported single-atom catalysts for nitrogen reduction reaction in a rapid way.Successfully,45 promising catalysts with highly efficient catalytic performance are screened out from 1626 candidates.Furthermore,based on the optimal feature sets,new catalytic descriptors are constructed via symbolic regression,which can be directly used to predict single-atom catalysts with good accuracy and good generalizability.This study not only provides dozens of promising catalysts and new descriptors for nitrogen reduction reaction but also offers a potential way for rapid screening of new electrocatalysts.

关键词： catalytic descriptor electrocatalytic nitrogen reduction first-principles calculations machine learning

FeTe_(2) as an earth-abundant metal telluride catalyst for electrocatalytic nitrogen fixation

在线全文

学校读者我要写书评

暂无评论

Journal of Energy Chemistry 2021年第5期30卷 259-263页

作者： Yali Guo Yonghua Cheng Qingqing Li Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina

Design of cost-effective,yet highly active electrocatalysts for nitrogen reduction reaction(NRR)is of vital significance for sustainable electrochemical NH_(3) synthesis.Herein,we have demonstrated,from both computational and experimental perspectives,that FeTe_(2) can be an efficient and durable NRR catalyst.Theoretical computations unveil that FeTe_(2) possesses abundant surface-terminated and low-coordinate Fe sites that can activate the NRR with a low limiting potential(-0.84 V)and currently impede the competing hydrogen evolution reaction.As a proof-of-concept prototype,we synthesized FeTe_(2) nanoparticles supported on reduced graphene oxide(FeTe_(2)/RGO),which exhibited a high NRR activity with the exceptional combination of NH_(3) yield(39.2 lg h^(-1) mg^(-1))and Faradaic efficiency(18.1%),thus demonstrating the feasibility of using FeTe_(2) and other earth-abundant metal tellurides for electrocatalytic N_(2) fixation.

关键词： electrocatalytic nitrogen reduction Fe catalysts Tellurides Density functional theory