检索结果-南通市图书馆

Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction

Nano-Micro Letters 2024年第1期16卷 55-67页

作者： zhaoyong Jin Meiqi Yang Yilong Dong Xingcheng Ma Ying Wang Jiandong Wu Jinchang Fan Dewen Wang Rongshen Xi Xiao zhao Tianyi Xu jingxiang zhao Lei Zhang David J.Singh Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEElectron Microscopy CenterJilin UniversityChangchun 130012People’s Republic of China Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of Educationand College of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025People’s Republic of China College of Chemistry Jilin UniversityChangchun 130012People’s Republic of China Department of Physics and Astronomy and Department of Chemistry University of MissouriColumbiaMO 65211USA

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.

关键词： CO_(2)reduction reaction Atomic dispersed catalyst Hetero-diatomic pair Ad-desorption energy Linear scaling relation

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Achieving efficient N_(2)electrochemical reduction by stabilizing the N2H*intermediate with the frustrated Lewis pairs

引用

Journal of Energy Chemistry 2022年第3期31卷 628-634,I0017页

作者： Zhe Chen jingxiang zhao Yan Jiao Tao Wang Lichang Yin Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025HeilongjiangChina Centre for Materials in Energy and Catalysis(CMEC) School of Chemical Engineering and Advanced MaterialsThe University of AdelaideAdelaideSA5005Australia Department of Physics and Electronic Information Huaibei Normal UniversityHuaibei 235000AnhuiChina

Electrocatalytic nitrogen reduction reaction(eNRR)with sustainable energy under ambient conditions represents an attractive approach to producing ammonia,but the design of the-state-of-the-art electrocatalyst with high efficiency and selectivity still faces formidable challenges.In contrast to traditional eNRR catalyst design strategies focusing on N≡N triple bond activation,we herein theoretically proposed an alternative strategy to improve eNRR performance via stabilizing the N_(2)H^(*)intermediate using catalysts with the frustrated Lewis pairs(FLPs),i.e.,transition metal(TM)atoms and boron(B)atom co-doped 2D black phosphorus(TM-B@BP).Our density functional theory(DFT)results reveal that the TM atom donates electrons to the adsorbed N_(2)molecule,while B atom provides empty orbital to stabilize the adsorption of N_(2)H^(*)intermediate.This framework successfully identifies five promising candidates(i.e.,Ti-B@BP,V-B@BP,Cr-B@BP,Mn-B@BP and Fe-B@BP)with low theoretical limiting potentials(−0.60,−0.41,−0.45,−0.43 and−0.50 V,respectively)and high selectivity for eNRR.We believe that the intermediate stabilization strategy introduced in current work offers a new opportunity to achieve accelerated and cost-effective ammonia synthesis with electrocatalysis.

关键词： Nitrogen reduction Electrocatalysis Intermediate stabilization strategy Density functional theory

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Efficient electrochemical reduction of CO to C_(2) products on the transition metal and boron co-doped black phosphorene

引用

Chinese Chemical Letters 2022年第4期33卷 2183-2187页

作者： Lingyi Kong Zhe Chen Qinghai Cai Lichang Yin jingxiang zhao College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024China Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety Harbin 150025China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Department of Physics and Electronic Information Huaibei Normal UniversityHuaibei 235000China

The synthesis of high-value multi-carbon products through the electrochemical reduction of carbon monoxide(COER) is one of the promising avenues for carbon utilization and energy storage,in which searching for efficient electrocatalysts that exhibit moderate CO intermediate binding strength and low kinetic barrier for C-C coupling is a key issue.Herein,by means of comprehensive density functional theory(DFT) computations,we theoretically designed three synergistic coupling catalysts by co-doping transition metal(TM=Fe,Co and Ni) and boron(B) into the two-dimensional black phosphorene(BP),namely TMB@BP for COER to C_(2) products.DFT computations and ab initio molecular dynamics simulations reveal the good stability and high feasibility of these proposed TM-B@BP catalysts for practical applications and future experimental synthesis.More interestingly,high-value ethylene(C_(2)H_(4)),ethane(C_(2)H_(6)) and ethanol(C_(2)H_(5)OH) products can be obtained on these three designed electrocatalysts with ultra-small limiting potentials(-0.20~-0.41 V) and low kinetic energy barriers of C-C coupling(0.52~0.91 eV).Meanwhile,the competitive one-carbon(C_(1)) products and hydrogen evolution reaction can also be effectively suppressed.The promising activity and selectivity of these three designed electrocatalysts render them ideal candidates for CO electroreduction,thus providing a cost-effective opportunity to achieve a sustainable production of high value C_(2) chemicals and fuels.

关键词： CO reduction Electrocatalysis Multi-carbon products Density functional theory 2D black phosphorene

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Applying machine-learning screening of single transition metal atoms anchored on N-dopedγ-graphyne for carbon monoxide electroreduction toward C_(1)products

引用

Nano Research 2023年第8期16卷 11511-11520页

作者： Dongxu Jiao Dantong Zhang Dewen Wang Jinchang Fan Xingcheng Ma jingxiang zhao Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control School of Materials Science and Engineeringand Key Laboratory of Automobile Materials of MOEJilin UniversityChangchun 130012China College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China Multiscale Crystal Materials Research Center Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China

Carbon monoxide electroreduction(COER)has been a key part of tandem electrolysis of carbon dioxide(CO_(2)),in which searching for high catalytic performance COER electrocatalysts remains a great challenge.Herein,by means of density functional theory(DFT)computations,we explored the potential of a series of transition metal atoms anchored on N-dopedγ-graphyne(TM@N-GY,TM from Ti to Au)as the COER electrocatalysts.We found that the final product selectivity of these single-atom catalysts depended on the position of the metal atom in the periodic table,with metals in the front and middle of each periodic period exhibiting high selectivity for CH_(4),while metals in the back producing CH_(3)OH.Machine learning(ML)found that metal atomic number was intrinsic to the difference in COER performance of these single-atom catalysts(SACs).The free energy changes showed that Mn@N-GY and Ni@N-GY exhibited outstanding COER catalytic performance for producing CH_(4)and CH_(3)OH,respectively.Our results provide theoretical and experimental guidance for designing efficient COER catalysts to generate C_(1)products.

关键词： CO electroreduction single atom catalysts γ-graphyne density functional theory machine learning

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Tuning precise numbers of supported nickel clusters on graphdiyne for efficient CO_(2)electroreduction toward various multi-carbon products

引用

Journal of Energy Chemistry 2022年第6期31卷 456-465,I0013页

作者： Meiqi Yang Zhongxu Wang Dongxu Jiao Yu Tian Yongchen Shang Lichang Yin Qinghai Cai jingxiang zhao College of Chemistry and Chemical Engineering Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025HeilongjiangChina Institute for Interdisciplinary Quantum Information Technology Jilin Engineering Normal UniversityChangchun 130052JilinChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety Harbin 150025HeilongjiangChina

Compared to single-atom catalysts,supported metal clusters can exhibit enhanced activity and designated selectivity in heterogeneous catalysis due to their unique geometric and electronic features.Herein,by means of comprehensive density functional theory (DFT) computations,we systematically investigated the potential of several Ni clusters supported on graphdiyne (Ni_(x)/GDY,x=1–6) for CO_(2) reduction reaction (CO_(2)RR).Our results revealed that,due to the strong interaction between Ni atoms and sp-hybridized C atoms,these supported Ni clusters on GDY exhibit high stabilities and excellent electronic properties.In particular,according to the computed free energy profiles for CO_(2)RR on these Ni_(x)/GDY systems,the anchored Ni_(4) cluster was revealed to exhibit high CO_(2)RR catalytic activity with a small limiting potential and moderate kinetic barrier for C–C coupling,and CH_(4),C_(2)H_(5)OH,and C_(3)H_(7)OH were identified as the main products,which can be attributed to its strong capacity for CO_(2) activation due to its unique configuration and excellent electronic properties.Thus,by carefully controlling the precise numbers of atoms in sub-nano clusters,the spatially confined Ni clusters can perform as promising CO_(2)RR catalysts with high-efficiency and high-selectivity,which may provide a useful guidance to further develop novel and low-cost metal clusters-based catalysts for sustain CO_(2)conversion to valuable chemicals and fuels.

关键词： CO_(2)reduction Supported metal clusters Graphdiyne Multi-carbon products Density functional theory

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Phthalocyanine-supported single-atom catalysts as a promising bifunctional electrocatalyst for ORR/OER: A computational study

引用

ChemPhysMater 2022年第3期1卷 237-245页

作者： Xinyi Li Zhongxu Wang Zhanhua Su Zhifeng zhao Qinghai Cai jingxiang zhao College of Chemistry and Chemical Engineering Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China College of Chemistry Guangdong University of Petrochemical TechnologyMaoming 525000China Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety Harbin 150025China

Developing excellent performance catalysts for the oxygen reduction reaction(ORR)and oxygen evolution re-action(OER)is fundamental for the commercialization of energy transduction and storage equipment.In our works,the potential of plenty of transition metals(TMs)anchored on phthalocyanine(TM-Pc)(TM=Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Mo,Ru,Rh,Pd,Ag,Re,Os,Ir,and Pt)as electrocatalysts for the ORR/OER was sys-tematically explored through synthetic density functional theory(DFT)computations.These TM-Pc candidates exhibited high electrochemical stability owing to the intense binding among the anchored TM and the Pc-based substrate.Interestingly,the free energy profiles showed that Ir-Pc can be performed as an outstanding bifunc-tional electrocatalyst for ORR/OER due to its ultralow overpotentials(𝜂ORR=0.46 V and𝜂OER=0.23 V),which can be reasonably explained by energetic and electronic descriptors.The present findings not only expand the database of single-atom catalysts(SACs),but also open the way for the reasonable design and development of advanced electrocatalysts for renewable energy technology.

关键词： Oxygen reduction/evolution Single-atom catalysts Phthalocyanine Density functional theory

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Two-dimensional Pt_(2)P_(3)monolayer:A promising bifunctional electrocatalyst with different active sites for hydrogen evolution and CO_(2)reduction

引用

Chinese Chemical Letters 2022年第8期33卷 3987-3992页

作者： Yuting Sun Shuang Wang Dongxu Jiao Fengyu Li Siyao Qiu Zhongxu Wang Qinghai Cai jingxiang zhao Chenghua Sun College of Chemistry and Chemical Engineering Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China School of Physical Science and Technology Inner Mongolia UniversityHohhot 010021China School of Chemical Engineering and Energy Technology Dongguan University of TechnologyDongguan 523808China Department of Chemistry and Biotechnology and Centre for Translational AtomaterialsSwinburne University of TechnologyHawthornVIC 3122Australia

Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)and CO_(2) electroreduction(CO_(2)ER)to valuable chemicals.Under such context,this work reported computational efforts to design promising electrocatalyst for HER and CO_(2)ER based on the swarm-intelligence algorithm.Among the family of transition-metal phosphides(TMPs),Pt_(2)P_(3) monolayer has been identified as excellent bifunctional catalysts due to high stability,excellent conductivity and superior catalytic performance.Different from typical d-block catalysts,p-band center presented by P atoms within Pt_(2)P_(3) monolayer plays the essential role for its reactivity towards HER and CO_(2)ER,underlining the key value of p-electrons in advanced catalyst design and thus providing a promising strategy to further develop novel catalysts made of p-block elements for various energy applications.

关键词： Bifunctional electrocatalysts HER/CO_(2)ER Swarm-intelligence structure search Density functional theory Two-dimensional Monolayer

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Ultrathin origami accordion-like structure of vacancy-rich graphitized carbon nitride for enhancing CO_(2) photoreduction

引用

Carbon Energy 2023年第4期5卷 94-104页

作者： Guangri Jia Zhongxu Wang Ming Gong Ying Wang Lu Hua Li Yilong Dong Lulu Liu Lei Zhang jingxiang zhao Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control Key Laboratory of Automobile Materials of MOESchool of Materials Science and EngineeringJilin UniversityChangchunJilinChina Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of EducationCollege of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbinHeilongjiangChina Institute for Frontier Materials Deakin UniversityWaurn PondsVictoriaAustralia College of Chemistry Jilin UniversityChangchunJilinChina

Retaining the ultrathin structure of two-dimensional materials is very important for stabilizing their catalytic performances.However,aggregation and restacking are unavoidable,to some extent,due to the van der Waals interlayer interaction of two-dimensional materials.Here,we address this challenge by preparing an origami accordion structure of ultrathin twodimensional graphitized carbon nitride(oa-C_(3)N_(4))with rich vacancies.This novel structured oa-C_(3)N_(4) shows exceptional photocatalytic activity for the CO_(2) reduction reaction,which is 8.1 times that of the pristine C_(3)N_(4).The unique structure not only prevents restacking but also increases light harvesting and the density of vacancy defects,which leads to modification of the electronic structure,regulation of the CO_(2) adsorption energy,and a decrease in the energy barrier of the carbon dioxide to carboxylic acid intermediate reaction.This study provides a new avenue for the development of stable highperformance two-dimensional catalytic materials.

关键词： C_(3)N_(4) CO_(2)photoreduction molecular modification photocatalysts solar energy conversion two-dimensional materials

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

N-heterocyclic carbene as a promising metal-free electrocatalyst with high efficiency for nitrogen reduction to ammonia

引用

Journal of Energy Chemistry 2020年第7期29卷 78-86,I0003页

作者： Hongyan Li Le Yang Zhongxu Wang Peng Jin jingxiang zhao Zhongfang Chen College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025HeilongjiangChina School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China Department of Chemistry University of Puerto RicoRio Piedras CampusSan JuanPR 00931USA

Electrocatalytic nitrogen reduction reaction(NRR)at ambient conditions holds great promise for sustainably synthesizing ammonia(NH3),while developing highly-efficient,long-term stable,and inexpensive catalysts to activate the inert N≡N bond is a key scientific issue.In this work,on the basis of the concept"N-heterocyclic carbenes(NHCs)",we propose a carbon decorated graphitic-carbon nitride(C/g-C3N4)as novel metal-free NRR electrocatalyst by means of density functional theory(DFT)computations.Our results reveal that the introduced C atom in g-C3N4 surface can be regarded as NHCs and catalytic sites for activating N≡N bond,and are stabilized by the g-C3N4 substrate due to sterically disfavored dimerization.Especially,this NHCs-based heterogeneous catalysis can efficiently reduce the activated N2 molecule to NH3 with a low overpotential of 0.05 V via an enzymatic mechanism.Our work is the first report of NHCs-based electrocatalyst for N2 fixation,thus opening an alternative avenue for advancing sustainable NH3 production.

关键词： Nitrogen reduction reaction N-heterocyclic carbenes Overpotential Density functional theory

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Single-atom rhodium anchored on S-doped black phosphorene as a promising bifunctional electrocatalyst for overall water splitting

引用

Chinese Chemical Letters 2023年第7期34卷 269-273页

作者： Xinyi Li Zhongxu Wang Yu Tian Xiaofeng Li Qinghai Cai jingxiang zhao College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin150025China Institute for Interdisciplinary Quantum Information Technology Jilin Engineering Normal UniversityChangchun 130052China Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety Harbin 150025China

Superior bifunctional electrocatalysts with ultra-high stability and excellent efficiency are crucial to boost the oxygen evolution reaction(OER) and the hydrogen evolution reduction(HER) in the overall water splitting(OWS) for the sustainable production of clean fuels. Herein, comprehensive density functional theory(DFT) computations were performed to explore the potential of several single transition metal(TM) atoms anchored on various S-doped black phosphorenes(TM/Snx-BP) for bifunctional OWS electrocatalysis. The results revealed that these candidates display good stability, excellent electrical conductivity, and diverse spin moments. Furthermore, the Rh/S12-BP catalyst was identified as an eligible bifunctional catalyst for OWS process due to the low overpotentials for OER(0.43 V) and HER(0.02 V), in which Rh and its adjacent P atoms were identified as the active sites. Based on the computed Gibbs free energies of OH~*, O~*, OOH~* and H~*, the corresponding volcano plots for OER and HER were established.Interestingly, the spin moments and the charge distribution of the active sites determine the catalytic trends of OER and HER. Our findings not only propose a promising bifunctional catalyst for OWS, but also widen the potential application of BP in electrocatalysis.

关键词： Overall water splitting Bifunctional catalysts Single-atom catalysts S-doped black phosphorene Density functional theory computations

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

欢迎您,

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

请选择保存的检索档案：

请选择收藏分类：

通借通还

欢迎您,

建议与咨询 留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

请选择保存的检索档案： 新增检索档案 确定 取消

请选择收藏分类： 新增自定义分类 确定 取消

通借通还

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

请选择保存的检索档案：

请选择收藏分类：