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1.
Adv Mater ; 36(21): e2313179, 2024 May.
Article in English | MEDLINE | ID: mdl-38353598

ABSTRACT

Single-atom decorating of Pt emerges as a highly effective strategy to boost catalytic properties, which can trigger the most Pt active sites while blocking the smallest number of Pt atoms. However, the rational design and creation of high-density single-atoms on Pt surface remain as a huge challenge. Herein, a customized synthesis of surface-enriched single-Bi-atoms tailored Pt nanorings (SE-Bi1/Pt NRs) toward methanol oxidation is reported, which is guided by the density functional theory (DFT) calculations suggesting that a relatively higher density of Bi species on Pt surface can ensure a CO-free pathway and accelerate the kinetics of *HCOOH formation. Decorating Pt NRs with dense single-Bi-atoms is achieved by starting from PtBi intermetallic nanoplates (NPs) with intrinsically isolated Bi atoms and subsequent etching and annealing treatments. The SE-Bi1/Pt NRs exhibit a mass activity of 23.77 A mg-1 Pt toward methanol oxidation in alkaline electrolyte, which is 2.2 and 12.8 times higher than those of Pt-Bi NRs and Pt/C, respectively. This excellent activity endows the SE-Bi1/Pt NRs with a high likelihood to be used as a practical anodic electrocatalyst for direct methanol fuel cells (DMFCs) with high power density of 85.3 mW cm-2 and ultralow Pt loading of 0.39 mg cm-2.

2.
ACS Nano ; 17(1): 402-410, 2023 Jan 10.
Article in English | MEDLINE | ID: mdl-36573959

ABSTRACT

High conversion efficiency over a wide operating potential window is important for the practical application of CO2 reduction electrocatalysis, yet that remains a huge challenge in differentiating the competing CO2 reduction and H2 evolution. Here we introduce point defects (Sn doping) and planar defects (grain boundary) into the Cu substrate. This multidimensional defect integration strategy guides the fabrication of highly diluted SnCu polycrystal, which exhibits high Faradaic efficiencies (>95%) toward CO2 electroreduction over an ultrawide potential window (ΔE = 1.3 V). The theoretical study indicates that the introduction of Sn doping and grain boundary synergistically provides an optimized electronic effect, which helps suppress H2 evolution and promotes the hydrogenation of *CO2.

3.
PLoS One ; 17(10): e0275717, 2022.
Article in English | MEDLINE | ID: mdl-36240231

ABSTRACT

In recent years, China's "lottery culture" has developed vigorously. Moreover, the investment participation rate of Chinese families in the formal financial market is low, whereas that in the informal financial market is high. Is there a certain relationship between "lottery culture" and family financial decision-making? If so, what is the underlying mechanism? Based on the 2017 CHFS data and lottery sales data of provinces, this study explores the impact of "lottery culture" on household participation in the formal and informal financial markets and the diversity of household financial portfolios. Results show that "lottery culture" can impede household participation in the formal financial market and the diversity of household financial portfolios while promoting household participation in the informal financial market in China. Furthermore, we analyze two channels of "lottery culture" impacts on household financial decisions: (1) risk attitude and (2) human capital. Results illustrate that "lottery culture" can influence household financial decisions by increasing risk tolerance and reducing the human capital of households.


Subject(s)
Family Characteristics , Investments , China , Humans
4.
Adv Mater ; 34(43): e2206276, 2022 Oct.
Article in English | MEDLINE | ID: mdl-36063819

ABSTRACT

The control of multimetallic ensembles at the atomic-level is challenging, especially for high-entropy alloys (HEAs) possessing five or more elements. Herein, the one-pot synthesis of hexagonal-close-packed (hcp) PtRhBiSnSb high-entropy intermetallic (HEI) nanoplates with intrinsically isolated Pt, Rh, Bi, Sn, and Sb atoms is reported, to boost the electrochemical oxidation of liquid fuels. Taking advantage of these combined five metals, the well-defined PtRhBiSnSb HEI nanoplates exhibit a remarkable mass activity of 19.529, 15.558, and 7.535 A mg-1 Pt+Rh toward the electrooxidation of methanol, ethanol, and glycerol in alkaline electrolytes, respectively, representing a state-of-the-art multifunctional electrocatalyst for alcohol oxidation reactions. In particular, the PtRhBiSnSb HEI achieves record-high methanol oxidation reaction (MOR) activity in an alkaline environment. Theoretical calculations demonstrate that the introduction of the fifth metal Rh enhances the electron-transfer efficiency in PtRhBiSnSb HEI nanoplates, which contributes to the improved oxidation capability. Meanwhile, robust electronic structures of the active sites are achieved due to the synergistic protections from Bi, Sn, and Sb sites. This work offers significant research advances in developing well-defined HEA with delicate control over compositions and properties.

5.
Small ; 18(14): e2107803, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35212141

ABSTRACT

Engineering multicomponent nanocatalysts is effective to improve electrocatalysis in many applications, yet it remains a challenge in constructing well-defined multimetallic active sites at the atomic level. Herein, the surface inlay of sub-monolayer Pb oxyhydroxide onto hexagonal PtBi intermetallic nanoplates with intrinsically isolated Pt atoms to boost the methanol oxidation reaction (MOR) is reported. The well-defined PtBi@6.7%Pb nanocatalyst exhibits 4.0 and 7.4 times higher mass activity than PtBi nanoplates and commercial Pt/C catalyst toward MOR in the alkaline electrolyte at 30 °C. Meanwhile, it also achieves a record-high mass activity of 51.07 A mg-1 Pt at direct methanol fuel cells operation temperature of 60 °C. DFT calculations reveal that the introduction of Pb oxyhydroxide on the surface not only promotes the electron transfer efficiency but also suppresses the CO poisoning effect, and the efficient p-d coupling optimizes the electroactivity of PtBi@6.7%Pb nanoplates toward the MOR process with low reaction barriers. This work offers a nanoengineering strategy to effectively construct and modulate multimetallic nanocatalysts to improve the electroactivity toward the MOR in future research.

6.
Adv Mater ; 33(17): e2008508, 2021 Apr.
Article in English | MEDLINE | ID: mdl-33749954

ABSTRACT

The rational design and control of electrocatalysts at single-atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi-Rh1 ) by atomic galvanic replacement, and their subsequent transformation into a tensile-strained Pt-Rh single-atom alloy (PtBi@PtRh1 ) via electrochemical dealloying are presented. Benefiting from the Rh1 -tailored Pt (110) surface with tensile strain, the PtBi@PtRh1 nanoplates exhibit record-high and all-round superior electrocatalytic performance including activity, selectivity, stability, and anti-poisoning ability toward ethanol oxidation in alkaline electrolytes. Density functional theory calculations reveal the synergism between effective Rh1 and tensile strain in boosting the adsorption of ethanol and key surface intermediates and the CC bond cleavage of the intermediates. The facile synthesis of the tensile-strained single-atom alloy provides a novel strategy to construct model nanostructures, accelerating the development of highly efficient electrocatalysts.

7.
Adv Mater ; 32(36): e2002822, 2020 Sep.
Article in English | MEDLINE | ID: mdl-32705724

ABSTRACT

Engineering novel Sn-based bimetallic materials could provide intriguing catalytic properties to boost the electrochemical CO2 reduction. Herein, the first synthesis of homogeneous Sn1- x Bix alloy nanoparticles (x up to 0.20) with native Bi-doped amorphous SnOx shells for efficient CO2 reduction is reported. The Bi-SnOx nanoshells boost the production of formate with high Faradaic efficiencies (>90%) over a wide potential window (-0.67 to -0.92 V vs RHE) with low overpotentials, outperforming current tin oxide catalysts. The state-of-the-art Bi-SnOx nanoshells derived from Sn0.80 Bi0.20 alloy nanoparticles exhibit a great partial current density of 74.6 mA cm-2 and high Faradaic efficiency of 95.8%. The detailed electrocatalytic analyses and corresponding density functional theory calculations simultaneously reveal that the incorporation of Bi atoms into Sn species facilitates formate production by suppressing the formation of H2 and CO.

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