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| 1 | Metal organic frameworks derived single atom catalysts for electrocatalytic energy conversion显示文摘The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to the maximum atom-utilization efficie ncy and unique electronic and geometric structures,single atom catalysts(SACs)have exhibited superior performance in various catalytic systems.Recently,assembled from the function alized orga nic lin kers and metal no des,metal-organic frameworks(MOFs)with ultrafi ne porosity have received treme ndous attention as precursors or self-sacrificing templates for preparing porous SACs.Here,the recent advances toward the synthesis strategies for using MOF precursors/templates to con struct SACs are systematically summarized with special emphasis on the types of central metal sites.The electrochemical applications of these recently emerged MOF-derived SACs for various energy-conversion processes,such as oxygen reduction/evolution reaction(ORR/OER),hydrogen evolution reaction(HER),and CO2 reduction reaction(CO2RR),are also discussed and reviewed.Fin ally,the curre nt challe nges and prospects regardi ng the developme nt of MOF-derived SACs are proposed. | Tingting Sun Lianbin Xu Dingsheng Wang Yadong Li | 2019 | Nano Research2019,12,9: | 63 |
| 2 | Insight of the stability and activity of platinum single atoms on ceria显示文摘Single-atom catalysts (SACs) have recently attracted broad attention in the catalysis field due to their maximized atom efficiency and unique catalytic properties.An atomic-level understanding of the interaction between the metal atoms and support is vital for developing stable and high-performance SACs.In this work,Pt1 single atoms with Ioadings up to 4 wt.% were fabricated on ceria nanorods using the atomic layer deposition technique.To understand the Pt-O-Ce bond interfacial interactions,the stability of Pt1 single atoms in the hydrogen reducing environment was extensively investigated by using in situ diffuse reflectance infrared Fourier transform spectroscopy CO chemisorption measurements.It was found that ceria defect sites,metal Ioadings and high-temperature calcination are effective ways to tune the stability of Pt1 single atoms in the hydrogen environment.X-ray photoemission spectroscopy further showed that Pt1 single atoms on ceria are dominantly at a +2 valence state at the defect and step edge sites,while those on terrace sites are at a +4 state.The above tailored stability and electronic properties of Pt1 single atoms are found to be strongly correlated with the catalytic activity in the dry and water-mediated CO oxidation reactions. | Xuxu Ye Hengwei Wang Yue Lin Xinyu Liu Lina Cao Jian Gu Junling Lu | 2019 | Nano Research2019,12,6: | 13 |
| 3 | Single titanium-oxide species implanted in 2D g-CsN4 matrix as a highly efficient visible-light CO2 reduction photocatalyst显示文摘A visible-light-response, efficie nt and robust photo-catalyst for CO2 reduction is highly desirable. Herein, we demonstrate that single titanium-oxide species impla nted in two-dime nsion al (2D) graphitic carb on n itride (g-C3N4) matrix (2D TiO-CN) can efficie ntly photo-catalyze the reduction of CO2 to CO under the irradiation of visible light. The synergistic interaction between single titanium oxide species and g-C3N4 in 2D TiO-CN not only enhances the separation of photo-excited charges, but also results in visible light response of single titanium-oxide species, realizing high activity of CO2 photo-reduction with extremely high CO generation rate of 283.9 pmol·h^-1·g^-1, 5.7, 6.8 and 292.2 times larger than those of TQ2/CN hybrid material, CN and commercial TiO2, respectively. Time-resolved fluoresce nee and electron spin resonance spectroscopy revealed the catalytic mechanism of the fabricated 2D TiO-CN photocatalysts for CO2 reduction. | Shangfeng Tang Xuepeng Yin Guanyu Wang Xiuli Lu Tongbu Lu | 2019 | Nano Research2019,12,2: | 8 |
| 4 | Recent advances in carbon-based electrocatalysts for oxygen reduction reaction显示文摘Fuel cells are one of the most promising clean energy devices to substitute for fossil fuel in the future to alleviate energy crisis and environmental pollution.As the key reaction on the cathode in the fuel cells,oxygen reduction reaction(ORR)still requires efficient noble metal catalysts such as the comme rcial Pt/C to boost the reaction for its sluggish kinetics.Therefore,it is critical to design earth-abundant carbonbased catalysts with high efficiency and long-term stability to replace the noble metal-based catalysts.This review focuses on the recent progress about carbon-based ORR catalysts including non-metal doped carbon materials,transition metal-nitrogen-carbon species,transition metal carbides/carbon,single atom catalysts,and other carbon hybrids.And we further infer that the excellent ORR performances can be achieved by the balance of geometric and electronic structures of catalysts such as conductivity,surface area,hierarchical porous structure,defect and doping effect.Additionally,the perspective development trend is also proposed to guide the rational designation of carbon-based catalysts for ORR and even extend to other energy storage and conversion fields in the future. | Lulu Chen Xiaolong Xu Wenxiu Yang Jianbo Jia | 2020 | Chinese Chemical Letters2020,31,3: | 5 |
| 5 | Single Atom Alloy Preparation and Applications in Heterogeneous Catalysis显示文摘There have been remarkable progresses in manipulating heterogeneous catalysts' nanostructures in the past decade.The concept of single atom alloy (SAA) was firstly proposed in 2012 when researchers successfully stabilized single Pd atoms on the Cu(111) surface.However,earlier work in 2009,which focused on replacing one Au atom with a Pd atom in thiolate protected Au25 nanoclusters,could also be considered as the pioneer work of single atom alloy.Both kinds of single atom alloys exhibited the potential of maximum utilization of scarce elements and attractive catalytic performances.The well-defined structures of SAA catalysts make accurate modeling possible,which further realizes the rational design of single atom alloy catalysts.In this review,we summarize the research trajectory of single atom alloys as well as recent achievements in this field.We also Introduce several commonly adopted characterization methods for SAA catalysts such as scanning tunneling microscopy (STM),temperature programmed reaction (TPR),extended X-ray absorption fine structure (EXAFS) spectra,matrix assisted laser desorption/ionization mass spectrum (MALDI-MS) and differential pulse voltammetry (DPV).Through discussing recent progresses in SAA catalysts,we propose that future researches in this filed should be focused on exploring new kinds of metal nanocrystals and controlling the nanostructure of SAA even more precisely. | Jianyu Han jjanmin Lu Min Wang Yehong Wang Feng Wang | 2019 | Chinese Journal of Chemistry2019,37,9: | 4 |
| 6 | A general bimetal-ion adsorption strategy to prepare nickel single atom catalysts anchored on graphene for efficient oxygen evolution reaction显示文摘Single-atom catalysts (SACs) supported on two-dimensional (2D) materials are highly attractive for maximizing their catalytic activity.However,graphene based SACs are primarily bonded with nitrogen and carbon sites,resulting in poor performance for the oxygen evolution reaction (OER).Herein,we develop a general bimetal-ion adsorption strategy for the synthesis of individually dispersed Ni SACs anchored on the oxygenated sites of ultrathin reduced graphene oxide as efficient OER electrocatalysts.The resultant Ni SACs for OER in alkaline electrolyte exhibit a highly stable overpotential of 328 mV at the current density of 10 mA cm^-2,and Tafel slope of 84 mV dec^-1 together with long-term durability and negligible degradation for 50 h,which is greatly outperform its counterparts of nitrogen bonded Ni SACs (564 mV,364 mV dec^-1) and Ni(OH)2 nanoparticles anchored on graphene (450 mV,142 mV dec^-1),and most reported Ni based OER electrocatalysts.Furthermore,the extended X-ray absorption fine structure at the Ni K-edge and theoretical simulation reveal that the nickel-oxygen coordination significantly boost OER performance.Therefore,this work will open numerous opportunities for creating novel-type 2D SACs via oxygen-metal bonding as highly robust OER catalysts. | Yingqi Xu Weifeng Zhang Yaguang Li Pengfei Lu Zhong-Shuai Wu | 2020 | Journal of Energy Chemistry2020,29,4: | 3 |
| 7 | Room-temperature conversion of ethane and the mechanism understanding over single iron atoms confined in graphene显示文摘The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane. | Suheng Wang Haobo Li Mengqi He Xiaoju Cui Lei Hua Haiyang Li Jianping Xiao Liang Yu N.Pethan Rajan Zhaoxiong Xie Dehui Deng | 2019 | Journal of Energy Chemistry2019,28,9: | 1 |