Supported metal-group materials are commonly utilized as state-of-the-art catalysts in industry.Atomic-sites catalysts(ASCs)have attracted increasing attention in catalysis owing to their 100%atom efficiency and uniqu...Supported metal-group materials are commonly utilized as state-of-the-art catalysts in industry.Atomic-sites catalysts(ASCs)have attracted increasing attention in catalysis owing to their 100%atom efficiency and unique catalytic performances toward various reactions.In particular,atomic dispersion of bulk and nano metals has become the focus of research and development in the synthesis of ASCs.Over the past decade,burgeoning interests have been paid to atomic dispersion in ASCs and their applications in catalysis.However,to the best of our knowledge,the systematic summary and analysis of atomic dispersion were rarely reported.In this review,recently developed ASCs by atomic dispersion were discussed in terms of synthetic atmosphere,driving force,applications in thermal catalytic reactions.Perspectives related to challenges and directions as well as design strategies of ASCs in atomic dispersion were also provided.展开更多
Developing highly active alloy catalysts that surpass the performance of platinum group metals in the oxygen reduction reaction(ORR)is critical in electrocatalysis.Gold-based single-atom alloy(AuSAA)clusters are gaini...Developing highly active alloy catalysts that surpass the performance of platinum group metals in the oxygen reduction reaction(ORR)is critical in electrocatalysis.Gold-based single-atom alloy(AuSAA)clusters are gaining recognition as promising alternatives due to their potential for high activity.However,enhancing its activity of AuSAA clusters remains challenging due to limited insights into its actual active site in alkaline environments.Herein,we studied a variety of Au_(54)M_(1) SAA cluster catalysts and revealed the operando formed MO_(x)(OH)_(y) complex acts as the crucial active site for catalyzing the ORR under the basic solution condition.The observed volcano plot indicates that Au_(54)Co_(1),Au_(54)M_(1),and Au_(54)Ru_(1) clusters can be the optimal Au_(54)M_(1) SAA cluster catalysts for the ORR.Our findings offer new insights into the actual active sites of AuSAA cluster catalysts,which will inform rational catalyst design in experimental settings.展开更多
We propose a scheme for the generation of the cluster states for many atoms in cavity QED.In our scheme,the atoms are sent through nonresonant cavity fields in the vacuum states.The cavity fields are only virtually ex...We propose a scheme for the generation of the cluster states for many atoms in cavity QED.In our scheme,the atoms are sent through nonresonant cavity fields in the vacuum states.The cavity fields are only virtually excitedand no quantum information will be transferred from the atoms to the cavity fields.The advantage is that the cavitiesare suppressed during the procedure.The scheme can also be generalized to the ion trap system.展开更多
Single atom catalysts(SATs)process the highest utilization efficiency of noble metals.The synergistic effect of noble single atoms and clusters,however,is insufficiently explored.In this work,Ru single atoms and clust...Single atom catalysts(SATs)process the highest utilization efficiency of noble metals.The synergistic effect of noble single atoms and clusters,however,is insufficiently explored.In this work,Ru single atoms and clusters are fabricated on CoP substrate simultaneously,using a facile synchronous phosphorization method,with pre-prepared CoOOH and RuCl_(3)mixture as the raw materials.It is demonstrated that strong charge transfer is established between Co and Ru elements,which leads to electron-sufficient Ru sites.As a result,the Ru species decorated CoP exhibits excellent electrocatalytic activity for HER,with an overpotential of 32 mV to afford a current density of 10 mA/cm^(2)and a Tafel slope of 37.6 mV/dec,much better than the pure CoP counterpart.This work provides insights into the exploration of synergistic effect of noble metal single atoms and clusters fabricated on transition metal phosphide substrate.展开更多
Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer...Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.展开更多
Catalytic reduction of dinitrogen to ammonia under mild conditions remains an attractive topic for the purpose of lowering energy consumption.Three-atom metal clusters have been proved an ideal model to explore highly...Catalytic reduction of dinitrogen to ammonia under mild conditions remains an attractive topic for the purpose of lowering energy consumption.Three-atom metal clusters have been proved an ideal model to explore highly efficient catalysts taking advantage of unique geometric/electronic structures and cooperative active sites.Here a study of N2 activation and reduction on seventeen bimetallic Nb_2M(M=Sc to Cu,and Y to Ag) clusters was reported.Three key processes for ammonia fixation(namely nitrogen activation,hydrogenation,and ammonia desorption) are fully studied,and three preferred systems(Nb_2Ni,Nb_2Rh and Nb_2Pd) are highlighted with outstanding catalytic performance.The d-σ and d-π~* orbital hybridizations between these metal clusters and N_(2) were demonstrated and the internal association with the N≡N bond activation was unveiled.By examining the ammonia synthesis on four chosen Nb_(2)M clusters(M=Fe,Ni,Rh and Pd),it can be elucidated that the distal pathway is more favorable than the alternative pathway in these systems.This work not only clarifies the N_(2) reduction on the bimetallic Nb_(2)M clusters,but also guides efficient bimetallic catalyst design.展开更多
This paper proposes two schemes to generate the multi-atom cluster states. The first scheme is based on the interaction of atoms with a highly detuned cavity mode and a classical field, the second scheme is based on t...This paper proposes two schemes to generate the multi-atom cluster states. The first scheme is based on the interaction of atoms with a highly detuned cavity mode and a classical field, the second scheme is based on the interaction of atoms with a cavity mode, strongly driven by a resonant classical field.展开更多
Three-dimensional distribution of solute elements in an Mg–Zn–Gd alloy during ageing process is quantitatively characterized by three-dimensional atom probe(3DAP) tomography. Based on the radius distribution functio...Three-dimensional distribution of solute elements in an Mg–Zn–Gd alloy during ageing process is quantitatively characterized by three-dimensional atom probe(3DAP) tomography. Based on the radius distribution function, it is found that Zn–Gd solute pairs in Mg matrix appear mainly at two peaks at early stage of ageing, and the separation distance between Zn and Gd atoms could be well rationalized by the first-principle calculation. Moreover, the fraction of Zn–Gd solute pairs increases first and then decreases due to the precipitation of long-period stacking ordered(LPSO) structures. Both the composition of the structural unit in LPSO structure and the solute enrichment around it are quantified. It is found that Zn and Gd elements are synchronized in the LPSO structure, and solute segregation of pure Zn or Gd is not observed at the transformation front of the LPSO structure in this alloy. In addition, the crystallography of transformation front is further determined by 3DAP data.展开更多
The investigation is generalized to clusters with sizes up to 3000 atoms, covering this way the range of sizes experimentally available for low energy cluster beam deposition. The atomic scale modeling is carried on b...The investigation is generalized to clusters with sizes up to 3000 atoms, covering this way the range of sizes experimentally available for low energy cluster beam deposition. The atomic scale modeling is carried on by both Molecular Dynamics and Metropolis Monte Carlo. This represents a huge series of simulations (175 cases) to which further calculations are added by spot when finer tuning of the parameters is necessary. Analyzing the results is a major task which is still in progress. This way, not only a realistic range of sizes is covered, but also the whole range of compositions and the temperature range relevant to the solid and the liquid states.展开更多
基金Japan Society of Promotion of Science(JSPS)(Nos.P21354 and P22049).
文摘Supported metal-group materials are commonly utilized as state-of-the-art catalysts in industry.Atomic-sites catalysts(ASCs)have attracted increasing attention in catalysis owing to their 100%atom efficiency and unique catalytic performances toward various reactions.In particular,atomic dispersion of bulk and nano metals has become the focus of research and development in the synthesis of ASCs.Over the past decade,burgeoning interests have been paid to atomic dispersion in ASCs and their applications in catalysis.However,to the best of our knowledge,the systematic summary and analysis of atomic dispersion were rarely reported.In this review,recently developed ASCs by atomic dispersion were discussed in terms of synthetic atmosphere,driving force,applications in thermal catalytic reactions.Perspectives related to challenges and directions as well as design strategies of ASCs in atomic dispersion were also provided.
文摘Developing highly active alloy catalysts that surpass the performance of platinum group metals in the oxygen reduction reaction(ORR)is critical in electrocatalysis.Gold-based single-atom alloy(AuSAA)clusters are gaining recognition as promising alternatives due to their potential for high activity.However,enhancing its activity of AuSAA clusters remains challenging due to limited insights into its actual active site in alkaline environments.Herein,we studied a variety of Au_(54)M_(1) SAA cluster catalysts and revealed the operando formed MO_(x)(OH)_(y) complex acts as the crucial active site for catalyzing the ORR under the basic solution condition.The observed volcano plot indicates that Au_(54)Co_(1),Au_(54)M_(1),and Au_(54)Ru_(1) clusters can be the optimal Au_(54)M_(1) SAA cluster catalysts for the ORR.Our findings offer new insights into the actual active sites of AuSAA cluster catalysts,which will inform rational catalyst design in experimental settings.
基金National Natural Science Foundation of China under Grant No.60478029
文摘We propose a scheme for the generation of the cluster states for many atoms in cavity QED.In our scheme,the atoms are sent through nonresonant cavity fields in the vacuum states.The cavity fields are only virtually excitedand no quantum information will be transferred from the atoms to the cavity fields.The advantage is that the cavitiesare suppressed during the procedure.The scheme can also be generalized to the ion trap system.
基金supported by the College Students Innovation and Entrepreneurship Training Program(202110350033)Science and Technology Innovation Project for College Students in Zhejiang Province(2021R436011).
文摘Single atom catalysts(SATs)process the highest utilization efficiency of noble metals.The synergistic effect of noble single atoms and clusters,however,is insufficiently explored.In this work,Ru single atoms and clusters are fabricated on CoP substrate simultaneously,using a facile synchronous phosphorization method,with pre-prepared CoOOH and RuCl_(3)mixture as the raw materials.It is demonstrated that strong charge transfer is established between Co and Ru elements,which leads to electron-sufficient Ru sites.As a result,the Ru species decorated CoP exhibits excellent electrocatalytic activity for HER,with an overpotential of 32 mV to afford a current density of 10 mA/cm^(2)and a Tafel slope of 37.6 mV/dec,much better than the pure CoP counterpart.This work provides insights into the exploration of synergistic effect of noble metal single atoms and clusters fabricated on transition metal phosphide substrate.
基金supported by the National Key Research and Development Program of China(2021YFA1500500,2019-YFA0405600)the CAS Project for Young Scientists in Basic Research(YSBR-051)+6 种基金the National Science Fund for Distinguished Young Scholars(21925204)the National Natural Science Foundation of China(22202192,U19A2015,22221003,22250007,22163002)the Collaborative Innovation Program of Hefei Science Center,CAS(2022HSCCIP004)the International Partnership,the DNL Cooperation Fund,CAS(DNL202003)the USTC Research Funds of the Double First-Class Initiative(YD9990002016,YD999000-2014)the Program of Chinese Academy of Sciences(123GJHZ2022101GC)the Fundamental Research Funds for the Central Universities(WK9990000095,WK999000-0124).
文摘Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.
基金financially supported by CAS Project for Young Scientists in Basic Research (No.YSBR-050)the National Natural Science Foundation of China (Nos.92261113 and 222721809)Beijing Natural Science Foundation (No.2232035)。
文摘Catalytic reduction of dinitrogen to ammonia under mild conditions remains an attractive topic for the purpose of lowering energy consumption.Three-atom metal clusters have been proved an ideal model to explore highly efficient catalysts taking advantage of unique geometric/electronic structures and cooperative active sites.Here a study of N2 activation and reduction on seventeen bimetallic Nb_2M(M=Sc to Cu,and Y to Ag) clusters was reported.Three key processes for ammonia fixation(namely nitrogen activation,hydrogenation,and ammonia desorption) are fully studied,and three preferred systems(Nb_2Ni,Nb_2Rh and Nb_2Pd) are highlighted with outstanding catalytic performance.The d-σ and d-π~* orbital hybridizations between these metal clusters and N_(2) were demonstrated and the internal association with the N≡N bond activation was unveiled.By examining the ammonia synthesis on four chosen Nb_(2)M clusters(M=Fe,Ni,Rh and Pd),it can be elucidated that the distal pathway is more favorable than the alternative pathway in these systems.This work not only clarifies the N_(2) reduction on the bimetallic Nb_(2)M clusters,but also guides efficient bimetallic catalyst design.
文摘This paper proposes two schemes to generate the multi-atom cluster states. The first scheme is based on the interaction of atoms with a highly detuned cavity mode and a classical field, the second scheme is based on the interaction of atoms with a cavity mode, strongly driven by a resonant classical field.
基金supported by a Grant-in-Aid for Scientific Research on Innovative Areas,‘‘Synchronized Long-Period Stacking Ordered Structure’’,from the Ministry of Education,Culture,Sports,Science and Technology,Japan(No.23109006)Fundamental Research Funds for the Central Universities(No.FRFTP-17-003A1)
文摘Three-dimensional distribution of solute elements in an Mg–Zn–Gd alloy during ageing process is quantitatively characterized by three-dimensional atom probe(3DAP) tomography. Based on the radius distribution function, it is found that Zn–Gd solute pairs in Mg matrix appear mainly at two peaks at early stage of ageing, and the separation distance between Zn and Gd atoms could be well rationalized by the first-principle calculation. Moreover, the fraction of Zn–Gd solute pairs increases first and then decreases due to the precipitation of long-period stacking ordered(LPSO) structures. Both the composition of the structural unit in LPSO structure and the solute enrichment around it are quantified. It is found that Zn and Gd elements are synchronized in the LPSO structure, and solute segregation of pure Zn or Gd is not observed at the transformation front of the LPSO structure in this alloy. In addition, the crystallography of transformation front is further determined by 3DAP data.
文摘The investigation is generalized to clusters with sizes up to 3000 atoms, covering this way the range of sizes experimentally available for low energy cluster beam deposition. The atomic scale modeling is carried on by both Molecular Dynamics and Metropolis Monte Carlo. This represents a huge series of simulations (175 cases) to which further calculations are added by spot when finer tuning of the parameters is necessary. Analyzing the results is a major task which is still in progress. This way, not only a realistic range of sizes is covered, but also the whole range of compositions and the temperature range relevant to the solid and the liquid states.
