Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
Oxygen evolution reaction(OER)catalysts face a major challenge in the practical implementation of acidic water electrolysis for hydrogen production,primarily due to limitations in catalytic activity and stability.Desp...Oxygen evolution reaction(OER)catalysts face a major challenge in the practical implementation of acidic water electrolysis for hydrogen production,primarily due to limitations in catalytic activity and stability.Despite extensive research,the development of acidic OER catalysts still relies largely on trial-and-error experimentation rather than AI-driven,target-oriented approaches.In this work,we address these limitations by introducing a spatial-adaptive active learning strategy integrated with closed-loop experimentation for targeted catalyst optimization in two stages.In the first stage,Bayesian optimization identifies highly active catalysts and a conditional variational autoencoder generates an adaptive low-overpotential subspace of stability candidates,while the second stage active learning finds the most stable catalyst within this subspace.Using this strategy,we discover a novel Cu-RuO_(2)catalyst that exhibits remarkable stability for 625 h and an overpotential of 177 mV at a current density of 10 mA cm^(−2).We provide detailed characterization and mechanistic insights into the newly discovered catalyst.Our study presents a transformative method for accelerating the design of stable acidic OER catalysts,thereby advancing the feasibility of large-scale green hydrogen production via acidic water electrolysis.展开更多
The scalable growth of wafer-sized single-crystal graphene in an energy-efficient manner and compatible with wafer process is critical for the killer applications of graphene in high-performance electronics and optoel...The scalable growth of wafer-sized single-crystal graphene in an energy-efficient manner and compatible with wafer process is critical for the killer applications of graphene in high-performance electronics and optoelectronics. Here, ultrafast epitaxial growth of single-crystal graphene wafers is realized on singlecrystal Cu90Ni10(1 1 1) thin films fabricated by a tailored two-step magnetron sputtering and recrystallization process. The minor nickel(Ni) content greatly enhances the catalytic activity of Cu, rendering the growth of a 4 in. single-crystal monolayer graphene wafer in 10 min on Cu90Ni10(1 1 1), 50 folds faster than graphene growth on Cu(1 1 1). Through the carbon isotope labeling experiments, graphene growth on Cu90Ni10(1 1 1) is proved to be exclusively surface-reaction dominated, which is ascribed to the Cu surface enrichment in the Cu Ni alloy, as indicated by element in-depth profile. One of the best benefits of our protocol is the compatibility with wafer process and excellent scalability. A pilot-scale chemical vapor deposition(CVD) system is designed and built for the mass production of single-crystal graphene wafers, with productivity of 25 pieces in one process cycle. Furthermore, we demonstrate the application of single-crystal graphene in electrically controlled liquid-crystal microlens arrays(LCMLA), which exhibit highly tunable focal lengths near 2 mm under small driving voltages. By integration of the graphene based LCMLA and a CMOS sensor, a prototype camera is proposed that is available for simultaneous light-field and light intensity imaging. The single-crystal graphene wafers could hold great promising for highperformance electronics and optoelectronics that are compatible with wafer process.展开更多
The present work employs a facile hydroxylation technique to efficiently functionalize the surface of a waste-derived aluminosilicate for ultra-high heavy metal uptake via ion exchange.The functionalization process le...The present work employs a facile hydroxylation technique to efficiently functionalize the surface of a waste-derived aluminosilicate for ultra-high heavy metal uptake via ion exchange.The functionalization process leads to the transformation of a nonporous hydrophobic waste material to a mesoporous hydrophilic material with a high concentration of ion exchange sites.The modification of the surface and textural characteristics of the mesoporous aluminosilicate has been thoroughly elucidated.The functionalization brings about the partial depolymerization of the aluminosilicate network and the transformation of unreactive bridging oxygens(BO)into non-bridging oxygens(NBO)as active sites as evidenced by^(29)Si NMR and FTIR.The positively-charged alkali metals bound to the NBO act as facile ion exchange sites.Ultra-high heavy metal uptake capacity of the functionalized material through a combination of ion exchange and physisorption mechanisms has revealed the great potential of this aluminosilicate material for treatment of heavy metal-laden wastewater in a sustainable manner for practical applications.展开更多
基金supported by the National Key R&D Program of China (2021YFA1502802)the National Natural Science Foundation of China (U21B2092, 22202213, 22402210, 22502215, 22502214, 22572200, and 22579171)+3 种基金the International Partnership Program of Chinese Academy of Sciences (172GJHZ2022028MI)the Shenyang Bureau of Science and Technology (24-213-3-25)the Natural Science Foundation of Liaoning Province (2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
基金supported by the National Natural Science Foundation of China(22502040 and 12374003)Shenzhen Basic Research Special Project(Natural Science Fund)Key Basic Research Project(JCYJ20241202123505008)+2 种基金Shenzhen Science and Technology Program(JCYJ20220531095208019 and GXWD20231129103124001)Guangzhou Municipal Science and Technology Project(2023A03J0003)Guangdong Basic and Applied Basic Research Foundation(2024A1515030256).
文摘Oxygen evolution reaction(OER)catalysts face a major challenge in the practical implementation of acidic water electrolysis for hydrogen production,primarily due to limitations in catalytic activity and stability.Despite extensive research,the development of acidic OER catalysts still relies largely on trial-and-error experimentation rather than AI-driven,target-oriented approaches.In this work,we address these limitations by introducing a spatial-adaptive active learning strategy integrated with closed-loop experimentation for targeted catalyst optimization in two stages.In the first stage,Bayesian optimization identifies highly active catalysts and a conditional variational autoencoder generates an adaptive low-overpotential subspace of stability candidates,while the second stage active learning finds the most stable catalyst within this subspace.Using this strategy,we discover a novel Cu-RuO_(2)catalyst that exhibits remarkable stability for 625 h and an overpotential of 177 mV at a current density of 10 mA cm^(−2).We provide detailed characterization and mechanistic insights into the newly discovered catalyst.Our study presents a transformative method for accelerating the design of stable acidic OER catalysts,thereby advancing the feasibility of large-scale green hydrogen production via acidic water electrolysis.
基金supported by the National Basic Research Program of China(2016YFA0200101 and 2014CB932500)the National Natural Science Foundation of China(21525310,51432002,51520105003,61432007,and 61176052)Beijing Municipal Science&Technology Commission(Z161100002116021 and Z181100004818001)
文摘The scalable growth of wafer-sized single-crystal graphene in an energy-efficient manner and compatible with wafer process is critical for the killer applications of graphene in high-performance electronics and optoelectronics. Here, ultrafast epitaxial growth of single-crystal graphene wafers is realized on singlecrystal Cu90Ni10(1 1 1) thin films fabricated by a tailored two-step magnetron sputtering and recrystallization process. The minor nickel(Ni) content greatly enhances the catalytic activity of Cu, rendering the growth of a 4 in. single-crystal monolayer graphene wafer in 10 min on Cu90Ni10(1 1 1), 50 folds faster than graphene growth on Cu(1 1 1). Through the carbon isotope labeling experiments, graphene growth on Cu90Ni10(1 1 1) is proved to be exclusively surface-reaction dominated, which is ascribed to the Cu surface enrichment in the Cu Ni alloy, as indicated by element in-depth profile. One of the best benefits of our protocol is the compatibility with wafer process and excellent scalability. A pilot-scale chemical vapor deposition(CVD) system is designed and built for the mass production of single-crystal graphene wafers, with productivity of 25 pieces in one process cycle. Furthermore, we demonstrate the application of single-crystal graphene in electrically controlled liquid-crystal microlens arrays(LCMLA), which exhibit highly tunable focal lengths near 2 mm under small driving voltages. By integration of the graphene based LCMLA and a CMOS sensor, a prototype camera is proposed that is available for simultaneous light-field and light intensity imaging. The single-crystal graphene wafers could hold great promising for highperformance electronics and optoelectronics that are compatible with wafer process.
文摘The present work employs a facile hydroxylation technique to efficiently functionalize the surface of a waste-derived aluminosilicate for ultra-high heavy metal uptake via ion exchange.The functionalization process leads to the transformation of a nonporous hydrophobic waste material to a mesoporous hydrophilic material with a high concentration of ion exchange sites.The modification of the surface and textural characteristics of the mesoporous aluminosilicate has been thoroughly elucidated.The functionalization brings about the partial depolymerization of the aluminosilicate network and the transformation of unreactive bridging oxygens(BO)into non-bridging oxygens(NBO)as active sites as evidenced by^(29)Si NMR and FTIR.The positively-charged alkali metals bound to the NBO act as facile ion exchange sites.Ultra-high heavy metal uptake capacity of the functionalized material through a combination of ion exchange and physisorption mechanisms has revealed the great potential of this aluminosilicate material for treatment of heavy metal-laden wastewater in a sustainable manner for practical applications.
