The single-pot production of Pd@Pt core-shell structures is a promising approach as it offers large surface area,catalytic capability,and stability.In this work,we established a single-pot process to produce Pd@Pt cor...The single-pot production of Pd@Pt core-shell structures is a promising approach as it offers large surface area,catalytic capability,and stability.In this work,we established a single-pot process to produce Pd@Pt core-shell nanodendrites with tunable composition,shape and size for optimal electrochemical activity.Pd@Pt nanodendrites with diverse compositions were synthesized by tuning the ratios of Pd and Pt sources in an aqueous environment using cetyltrimethylammonium chloride,which functioned as both the surfactant and the reducing agent at an elevated temperature(90°C).The synthesized Pd5@Pt5 nanodendrites showed exceptional electrochemical action toward the methanol oxidation reaction related with another compositional Pd@Pt nanodendrites and conventional Pt/C electrocatalysts.In addition,Pd5@Pt5 nanodendrites exhibited good CO tolerance owing to their surface features and the synergistic effect among Pt and Pd.Meanwhile,nanodendrites with a Pt-rich surface provided exceptional catalytic active sites.Compared with the conventional Pt/C electrocatalyst,the anodic peak current obtained by Pd5@Pt5 nanodendrites was 3.74 and 2.18 times higher in relations of mass and electrochemical active surface area-normalized current density,respectively.This approach offers an attractive strategy to design electrocatalysts with unique structures and outstanding catalytic performance and stability for electrochemical energy conversion.展开更多
A power-law (y = cx<sup>n</sup>) signature between process energy budget (kJ) and process energy density (kJ·ml<sup>-1</sup>) of microwave-assisted synthesis of silver and gold nanostructu...A power-law (y = cx<sup>n</sup>) signature between process energy budget (kJ) and process energy density (kJ·ml<sup>-1</sup>) of microwave-assisted synthesis of silver and gold nanostructures has been recently described [Law and Denis. AJAC, 14(4), 149-174, (2023)]. This study explores this relation further for palladium, platinum, and zinc oxide nanostructures. Parametric cluster analysis and statistical analysis is used to test the power-law signature of over four orders of magnitude as a function of six microwave applicator-types metal precursor, non-Green Chemistry synthesis and claimed Green Chemistry. It is found that for the claimed Green Chemistry, process energy budget ranges from 0.291 to 900 kJ, with a residual error ranging between −33 to +25.9 kJ·ml<sup>-1</sup>. The non-Green Chemistry synthesis has a higher process energy budget range from 3.2 kJ to 3.3 MJ, with a residual error of −33.3 to +245.3 kJ·ml<sup>-1</sup>. It is also found that the energy profile over time produced by software controlled digestion applicators is poorly reported which leads to residual error problematic outliers that produce possible phase-transition in the power-law signature. The original Au and Ag database and new Pd, Pt and ZnO database (with and without problematic outliers) yield a global microwave-assisted synthesis power-law signature constants of c = 0.7172 ± 0.3214 kJ·ml<sup>-1</sup> at x-axes = 0.001 kJ, and the exponent, n = 0.791 ± 0.055. The information in this study is aimed to understand variations in historical microwave-assisted synthesis processes, and develop new scale-out synthesis through process intensification.展开更多
基金the Basic Science Research Program of the National Research Foundation(NRF)of Korea(Nos.2019R1A6A1A11053838,2022R1A4A3033528,and 2022R1F1A1063285)Korea Agency for Infrastructure Technology Advancement(KAIA)funded by the Ministry of Land,Infrastructure,and Transport(No.21CTAP-C163795-01)Prof.M.Y.Choi acknowledges the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(Nos.2019R1A6C1010042 and 2021R1A6C103A427).
文摘The single-pot production of Pd@Pt core-shell structures is a promising approach as it offers large surface area,catalytic capability,and stability.In this work,we established a single-pot process to produce Pd@Pt core-shell nanodendrites with tunable composition,shape and size for optimal electrochemical activity.Pd@Pt nanodendrites with diverse compositions were synthesized by tuning the ratios of Pd and Pt sources in an aqueous environment using cetyltrimethylammonium chloride,which functioned as both the surfactant and the reducing agent at an elevated temperature(90°C).The synthesized Pd5@Pt5 nanodendrites showed exceptional electrochemical action toward the methanol oxidation reaction related with another compositional Pd@Pt nanodendrites and conventional Pt/C electrocatalysts.In addition,Pd5@Pt5 nanodendrites exhibited good CO tolerance owing to their surface features and the synergistic effect among Pt and Pd.Meanwhile,nanodendrites with a Pt-rich surface provided exceptional catalytic active sites.Compared with the conventional Pt/C electrocatalyst,the anodic peak current obtained by Pd5@Pt5 nanodendrites was 3.74 and 2.18 times higher in relations of mass and electrochemical active surface area-normalized current density,respectively.This approach offers an attractive strategy to design electrocatalysts with unique structures and outstanding catalytic performance and stability for electrochemical energy conversion.
文摘A power-law (y = cx<sup>n</sup>) signature between process energy budget (kJ) and process energy density (kJ·ml<sup>-1</sup>) of microwave-assisted synthesis of silver and gold nanostructures has been recently described [Law and Denis. AJAC, 14(4), 149-174, (2023)]. This study explores this relation further for palladium, platinum, and zinc oxide nanostructures. Parametric cluster analysis and statistical analysis is used to test the power-law signature of over four orders of magnitude as a function of six microwave applicator-types metal precursor, non-Green Chemistry synthesis and claimed Green Chemistry. It is found that for the claimed Green Chemistry, process energy budget ranges from 0.291 to 900 kJ, with a residual error ranging between −33 to +25.9 kJ·ml<sup>-1</sup>. The non-Green Chemistry synthesis has a higher process energy budget range from 3.2 kJ to 3.3 MJ, with a residual error of −33.3 to +245.3 kJ·ml<sup>-1</sup>. It is also found that the energy profile over time produced by software controlled digestion applicators is poorly reported which leads to residual error problematic outliers that produce possible phase-transition in the power-law signature. The original Au and Ag database and new Pd, Pt and ZnO database (with and without problematic outliers) yield a global microwave-assisted synthesis power-law signature constants of c = 0.7172 ± 0.3214 kJ·ml<sup>-1</sup> at x-axes = 0.001 kJ, and the exponent, n = 0.791 ± 0.055. The information in this study is aimed to understand variations in historical microwave-assisted synthesis processes, and develop new scale-out synthesis through process intensification.
