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atomically dispersed catalysts for small molecule electrooxidation in direct liquid fuel cells

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Journal of Energy Chemistry 2022年第5期31卷 439-453页

作者： Jinfa Chang Guanzhi Wang Wei Zhang Yang Yang NanoScience Technology Center University of Central FloridaOrlandoFL 32826USA Department of Materials Science and Engineering University of Central FloridaOrlandoFL 32826USA Department of Chemistry Renewable Energy and Chemical Transformation ClusterUniversity of Central FloridaOrlandoFL 32826USA

Direct liquid fuel cells(DLFCs) have received increasing attention because of their high energy densities,instant recharging abilities, simple cell structure, and facile storage and transport. The main challenge for the commercialization of DLFCs is the high loading requirement of platinum group metals(PGMs) as catalysts. atomically dispersed catalysts(ADCs) have been brought into recent focus for DLFCs due to their well-defined active sites, high selectivity, maximal atom-utilization, and anti-poisoning property. In this review, we summarized the structure–property relationship for unveiling the underlying mechanisms of ADCs for DLFCs. More specifically, different types of fuels used in DLFCs such as methanol, formic acid,and ethanol were discussed. At last, we highlighted current challenges, research directions, and future outlooks towards the practical application of DLFCs.

关键词： atomic dispersion Electrocatalyst Small molecule electrooxidation Direct liquid fuel cells

Single-atom Zn for boosting supercapacitor performance

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Nano Research 2022年第3期15卷 1715-1724页

作者： Zongge Li Danni Wang Huifang Li Mang Ma Ying Zhang Zifeng Yan Stefano Agnoli Guoxin Zhang Xiaoming Sun State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China Al-ion Battery Research Center Department of Electrical Engineering and AutomationShandong University of Science and TechnologyQingdao 266590China State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Department of Chemical Sciences University of PadovaVia Marzolo 1Padova I-35131Italy College of Electromechanical Engineering Shandong Engineering Laboratory for Preparation and Application of High-performance CarbonMaterialsQingdao University of Science&TechnologyQingdao 266061China

Single-atom metal-incorporated carbon nanomaterials(CMs)have shown great potential towards broad catalytic *** this work,we show that N-doped porous CMs embedded with redox-able Zn atoms exhibit superior capacitive *** Zn(~2.72 at.%)/N(~12.51 at.%)doping were realized by incorporating Zn2+and benzamide into the condensation and carbonization of formamide and subsequent annealing at 900℃.The Zn and N species are mutually benefited during the formation of ZnN4 *** as-obtained Zn1NC material affords a very large capacitance of 621 F·g^(−1)(at 0.1 A·g^(−1)),superior rate capability(~65%retention at 100 A·g^(−1)),and excellent cycling stability(0.00044%per cycle at 10 A·g^(−1)).These merits are attributed to the high Zn/N loading,atomic Zn-boosted pseudocapacitive behavior,large specific surface area(~1,085 m^(2)·g^(−1)),and rich pore hierarchy,thus ensuring both large pseudo-capacitance(e.g.,~37.9%at 10 mV·s^(−1))and double-layer *** of establishing a new type of high Zn/N-loading carbon materials,our work uncovers the capacitive roles of atomically dispersed metals in CMs.

关键词： atomic dispersion zinc doping nitrogen doping carbon nanomaterial supercapacitor

A Universal Principle to Accurately Synthesize atomically Dispersed Metal–N_4 Sites for CO_2 Electroreduction

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Nano-Micro Letters 2020年第9期12卷 14-25页

作者： Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China College of Geography and Environmental Science Zhejiang Normal UniversityJinhua 321004People’s Republic of China College of Environment Zhejiang University of TechnologyHangzhou 310014People’s Republic of China Institute of Zhejiang University-Quzhou Quzhou 324000People’s Republic of China Ningbo Research Institute Zhejiang UniversityNingbo 315100People’s Republic of China Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

atomically dispersed metal-nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction(CO2 ER),but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central ***,we develop a family of single metal atom bonded by N atoms anchored on carbons(SAs-M-N-C,M=Fe,Co,Ni,Cu)for CO2 ER,which composed of accurate pyrrole-type M-N4 structures with isolated metal atom coordinated by four pyrrolic N *** from atomically coordinated environment and specific selectivity of M-N4 centers,SAs-Ni-N-C exhibits superior CO2 ER performance with onset potential of-0.3 V,CO Faradaic efficiency(F.E.) of 98.5%at-0.7 V,along with low Tafel slope of 115 mV dec-1 and superior stability of 50 h,exceeding all the previously reported M-N-C electrocatalysts for CO2-to-CO *** results manifest that the different intrinsic activities of M-N4 structures in SAs-M-N-C result in the corresponding sequence of Ni> Fe> Cu> Co for CO2 ER *** integrated Zn-CO2 battery with Zn foil and SAs-Ni-N-C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output,which delivers a peak power density of 1.4 mW cm-2 and maximum CO *** 93.3%.

关键词： atomic dispersion Pyrrole-type metal–N4 structure Catalytic site CO2 electroreduction Zn–CO2 battery

atomic iron on mesoporous N-doped carbon to achieve dehydrogenation reaction at room temperature

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Nano Research 2020年第11期13卷 3075-3081页

作者： Zheng Chen Wenjuan Yang Yue Wu Chao Zhang Jun Luo Chen Chen Yadong Li Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Key Laboratory of Molecule-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu241000China International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen518060China Department of Chemistry Tsinghua UniversityBeijing100084China View author publications Center for Electron Microscopy Tianjin University of TechnologyTianjin300384China

atomic non-noble metal materials show the potential to substitute noble metals in ***,melamine formaldehyde resin is developed to synthesize atomic iron on mesoporous nitrogen-doped *** triazine units with abundant nitrogen content and cavity can realize effectively anchoring of single metal *** atomic iron with unique charge and coordination characteristics shows superior catalytic performance in dehydrogenation *** N-heterocycles compounds and amines can be efficiently dehydrogenated into the corresponding products at room temperature,which is the mildest of all reported reaction conditions even when noble metal catalysts are ***,development of atomic non-noble metal catalysts with mesoporous structure may provide an effective way to realize the substitution for noble metals in heterogeneous catalysis.

关键词： atomic dispersion non-noble metal nitrogen-doped carbon mesoporous structure dehydrogenation

Rational design of palladium single-atoms and clusters supported on silicoaluminophosphate-31 by a photochemical route for chemoselective hydrodeoxygenation of vanillin

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Nano Research 2021年第11期14卷 4347-4355页

作者： Xiaowen Lu Chunmu Guo Mingyang Zhang Leipeng Leng J.Hugh Horton Wei Wu Zhijun Li Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing163318China National Center for International Research on Catalytic Technology School of Chemistry and Material ScienceHeilongjiang UniversityHarbin150080China Department of Chemistry Queen’s UniversityKingstonK7L 3N6Canada

Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added ***,we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31(SAPO-31)as a highly active,chemoselective,and reusable catalyst for hydrodeoxygenation of *** by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy,extended X-ray absorption fine structure measurement,and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed,without forming strong palladium-palladium metallic bonding,over the SAPO-31 *** catalyst,with a full metal availability to the reactants,exhibits exceptional catalytic activity(TOF:3,000 h^(−1),Yield:>99%)in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol(MMP)under mild conditions(1 atm,80°C,30 min),along with excellent stability,scalability(up to 100-fold),and wide substrate *** superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters,as well as the strong metal-support *** work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.

关键词： heterogeneous catalysis photochemical reduction palladium single atoms and clusters atomic dispersion hydrodeoxygenation vanillin

Boosting the Ni-Zn interplay via O/N dual coordination for high-efficiency CO_(2) electroreduction

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Carbon Energy 2023年第4期5卷 68-80页

作者： Ying Zhang Hailei Jiang Anuj Kumar Hongchuan Zhang Zongge Li Tongxin Xu Yuan Pan Yaqun Wang Zhiming Liu Guoxin Zhang Zifeng Yan State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)QingdaoShandongChina Department of Chemistry Institute of Humanities and Applied ScienceGLA UniversityMathuraIndia College of Chemistry and Chemical Engineering Liaocheng UniversityLiaochengShandongChina Al‐Ion Battery Research Center College of Energy Storage TechnologyShandong University of Science and TechnologyQingdaoShandongChina Shandong Engineering Laboratory for Preparation and Application of High‐performance Carbon‐Materials College of Electromechanical EngineeringQingdao University of Science and TechnologyQingdaoShandongChina

Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction of CO_(2) to value-added fuels and chemicals and to achieving carbon ***,atomic Ni(Zn)sites that are uniquely coordinated with ternary Zn(Ni)/N/O ligands were successfully decorated on formamide-derived porous carbon nanomaterials,possibly forming an atomic structure of Ni(N_(2)O_(1))-Zn(N_(2)O_(1)),as studied by combining X-ray photoelectron spectroscopy and X-ray absorption *** the mediation of additional O coordination,the Ni-Zn dual site induces significantly decreased desorption of molecular *** NiZn-NC decorated with rich Ni(N_(2)O_(1))-Zn(N_(2)O_(1))sites remarkably gained>97%CO Faraday efficiency over a wide potential range of -0.8 to -1.1 V(relative to reversible hydrogen electrode).Density functional theory computations suggest that the N/O dual coordination effectively modulates the electronic structure of the Ni-Zn duplex and optimizes the adsorption and conversion properties of CO_(2) and subsequent *** from the conventional pathway of using Ni as the active site in the Ni-Zn duplex,it is found that the Ni-neighboring Zn sites in the Ni(N_(2)O_(1))-Zn(N_(2)O_(1))coordination showed much lower energy barriers of the CO_(2) protonation step and the subsequent dehydroxylation step.

关键词： atomic dispersion carbon materials CO_(2)reduction formamide metal-nitrogen-carbon

Topotactic reduction of layered double hydroxides for atomically thick two-dimensional non-noble-metal alloy

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Nano Research 2017年第9期10卷 2988-2997页

作者： Pengsong Li Qixian Xie Lirong Zheng Guang Feng Yingjie Li Zhao Cai Yongmin Bi Yaping Li Yun Kuang Xiaoming Sun Xue Duan State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 China College of Energy Beijing University of Chemical Technology Beijing 100029 China Beijing Advanced Innovation Centre for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

Layered double hydroxides (LDHs) have been widely used as catalysts owing to their tunable structure and atomic dispersion of high-valence metal ions; however, limited tunability of electronic structure and valence states have hindered further improvement in their catalytic performance. Herein, we reduced ultrathin LDH precursors in situ and topotactically converted them to atomically thick (~2 nm) two-dimensional (2D) multi-metallic, single crystalline alloy nanosheets with highly tunable metallic compositions. The as-obtained alloy nanosheets not only maintained the vertically aligned ultrathin 2D structure, but also inherited the atomic dispersion of the minor metallic compositions of the LDH precursors, even though the atomic percentage was higher than 20%, which is far beyond the reported percentages for single-atom dispersions (usually less than 0.1%). Besides, surface engineering of the alloy nanosheets can finely tune the surface electronic structure for catalytic applications. Such in situ topotactic conversion strategy has introduced a novel approach for atomically dispersed alloy nanostructures and reinforced the synthetic methodology for ultrathin 2D metal-based catalysts.

关键词： atomic thickness two-dimensional (2D) nanosheets non-noble-metal alloy atomic dispersion catalysis

In situ thermal-induced generation of{Ag^(0)Ag^(Ⅰ)}dimer within Co-Ag phosphonates

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Chinese Chemical Letters 2022年第6期33卷 3259-3262页

作者： Qingqing Guo Nanzhu Li Qian Zou Jiage Jia Yifan Wei Songsong Bao Limin Zheng State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

The thermal decomposition of Ag NO_(3)is known to produce metallic Ag,but single-atomic dispersion is hard to achieve instead of the aggregation state of ***,we develop an efficient approach to thermally generate and stabilize single Ag atoms via the coordination *** desired Co-Ag phosphonates[Ag_(2)^(Ⅰ)Co_(2)^(Ⅲ)(notp H_(3))_2(NO_(3))]X[X=NO_(3)^(-)(1)or Cl O_(4)^(-)(2)]were synthesized by solid-phase grinding method or solution *** crystal structures reveal slightly different packing arrangements of various lattice anions and identical one-dimensional(1-D)coordination chains,formed in each case by the coordination of Ag(Ⅰ)to the metalloligand Co(notp H_(3))and NO_(3)^(-) *** number of Ag(Ⅰ)ions connected to each NO_(3)^(-) anion reduces from 5 in bulk Ag NO_(3) to 2 in compounds 1 and 2,leading to the Ag NO_(3)component stepwise decomposition at a lower temperature(<300℃).During the thermal decomposition,the changes of supermolecular structures and Ag oxidation states were monitored by PXRD,IR and XAFS *** most interesting finding is that 1 and 2 can retain chain structures and harvest Ag(0)atoms in the chain by controlling decomposition temperatures(220℃for 1 and 254℃for 2).

关键词： Metallic silver Thermal decomposition Metal phosphonate atomic dispersion Magnetism

Top-down synthesis strategies: Maximum noble-metal atom efficiency in catalytic materials

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Chinese Journal of Catalysis 2017年第9期38卷 1588-1596页

作者： Yaxin Chen Zhiwei Huang Xiao Gu Zhen Ma Jianmin Chen Xingfu Tang Institute of Atmospheric Sciences Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention (LAP3) Department of Environmental Science & Engineering Fudan University Shanghai 200433 China Department of Applied Physics Chongqing University Chongqing 401331 China Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET) Nanjing University of Information Science & Technology Nanjing 210044 Jiangsu China

Top‐down synthesis has been used to prepare catalytic materials with nanometer sizes,but fabricating atomically dispersed metal catalysts remains a challenge because surface single metal atoms are prone to aggregation or coalescence.A top‐down strategy is used to synthesize atomically dispersed metal catalysts,based on supported Ag *** changes of the geometric and electronic structures of the Ag atoms during the top‐down process are studied using the in situ synchrotron X‐ray diffraction technique,ex situ X‐ray absorption spectroscopy,and transmission electron *** experimental results,coupled with the density functional theory calculations,demonstrate that the electronic perturbation of the Ag frontier orbitals,induced by the Ag‐O interactions at the perimeter of the metal‐support interface,is the driving force of the top‐down *** top‐down synthesis has two important functions:to increase the number of catalytic active sites and to facilitate the study of complex reaction mechanisms(e.g.,formaldehyde oxidation)by developing single‐site model catalysts.

关键词： Top‐down synthesis atomic dispersion Catalytic active site Electronic metal‐support interaction Formaldehyde oxidation