Trace Pd modified intermetallic PtBi nanoplates towards efficient formic acid electrocatalysis

Tang, Min; Chen, Wen; Luo, Shuiping; Wu, Xiaotong; Fan, Xiaokun; Liao, Yujia; Song, Xing; Cheng, Yu; Li, Lanxi; Tan, Li; Liu, Yulian; Quan, Zewei

doi:10.1039/d1ta01123e

Cited by 41 publications

(21 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…[17,[21][22][23][24] On the other hand, surface modification of Pt nanocrystals via adatoms, deposited atoms, or doped atoms significantly improve the electrocatalytic properties due to the geometric and electronic effects, but unfortunately, the active sites involved are usually distributed randomly. [25][26][27][28][29][30][31][32][33][34][35][36] Therefore, engineering multicomponent nanocatalyst by combining the isolation and surface modification of Pt atoms via certain metals is expected to produce highly efficient Pt-based electrocatalysts toward MOR.…”

Section: Introductionmentioning

confidence: 99%

Hexagonal PtBi Intermetallic Inlaid with Sub‐Monolayer Pb Oxyhydroxide Boosts Methanol Oxidation

Chen

Luo

Sun

et al. 2022

Small

Self Cite

View full text Add to dashboard Cite

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–1Pt 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.

show abstract

Section: Introductionmentioning

confidence: 99%

Hexagonal PtBi Intermetallic Inlaid with Sub‐Monolayer Pb Oxyhydroxide Boosts Methanol Oxidation

Chen

Luo

Sun

et al. 2022

Small

Self Cite

View full text Add to dashboard Cite

show abstract

“…presented a deposition method to construct a core‐shell structure based on the PtM intermetallic. [ 39 ] Briefly, trace Pd atoms (1.8 at%) were introduced to optimize the surface of intermetallic PtBi nanoplates, which contributed to the formation of tensile‐strained Pd and electronic‐modulated intermetallic PtBi. Due to the synergistic effect between the PtBi intermetallic and Pd atoms, enhanced formic acid oxidation activity was achieved.…”

Section: Optimization Strategies For Structurally Ordered Materialsmentioning

confidence: 99%

Recent Progress on Structurally Ordered Materials for Electrocatalysis

Sun

Song

et al. 2021

Advanced Energy Materials

View full text Add to dashboard Cite

Tuning material properties by modulation of the arrangement of atoms is a fundamental and effective strategy in materials science. Structurally long‐range ordered materials are increasingly finding utility for electrocatalytic applications. Such ordered structures can achieve unique functions that increase the electrocatalytic activity compared to corresponding electrocatalysts with a disordered structure. Effective strategies for designing high‐performance electrocatalysts based on structurally ordered materials are presented. This review also summarizes the recent progress on structurally ordered materials as efficient electrocatalysts and highlights the applications in several representative electrochemical reactions, such as, the oxygen evolution reaction, oxygen reduction reaction, and hydrogen evolution reaction. The structural features of the atomic long‐range ordered framework and superior electrochemical performance are demonstrated by advanced characterization techniques (structural identification) and electrochemical measurements (performance evaluations), respectively. Special attention is paid to the establishment of a structure‐activity relationship to highlight the advantages of the ordered structure. Finally, the remaining challenges and emerging opportunities in these related materials are proposed.

show abstract

“…The mass activity was 69.3 A mg Pt −1 , which places the nanoplates among the best catalysts reported so far (Table S3, Supporting Information). [18,[29][30][31][32][33][34][35][36][37] It is worth noting that the Ag@Au@Pt 0.26L nanoplates also show a high mass activity normalized to the total mass of the metals (0.811 A mg Au+Ag+Pt ), which is 7.8 times greater than that of the commercial Pt/C, suggesting a high potential of these catalysts in practical applications (Figure S16, Supporting Information).…”

Section: Electrocatalytic Performance Of the Catalysts In The Faormentioning

confidence: 99%

Ligand‐Mediated Self‐Terminating Growth of Single‐Atom Pt on Au Nanocrystals for Improved Formic Acid Oxidation Activity

Liu

Xie

et al. 2021

Advanced Energy Materials

View full text Add to dashboard Cite

acid oxidation reaction (FAOR) and many other important heterogeneous catalytic reactions. [5][6][7][8][9][10][11][12][13] A dual-path mechanism has been proposed for the FAOR based on experiments and theory, i.e., a direct path that involves the dehydrogenation of HCOOH directly to CO 2 , and an indirect path that involves the dehydration of HCOOH to CO 2 via a poisoning intermediate of CO. [5][6][7][8] The direct path is preferred because it bypasses the formation of CO that easily poisons the catalyst. It is recognized that the reaction paths of the FAOR can be effectively regulated by the ensemble size of the Pt catalyst. The direct and indirect paths of the FAOR occur at isolated single atoms and large ensembles of Pt, respectively. [5][6][7][8] Therefore, Pt catalysts with the smallest ensemble size, i.e., isolated single atoms, are among the most active catalysts for this reaction.However, it is difficult to reliably construct isolated single atoms of Pt on a foreign metal substrate in a wet-chemical synthesis, because the formation of large ensembles or islands of Pt is an energetically more favorable process owing to the high Pt-Pt bond energy. [14][15][16][17] It is only possible to maintain isolated single atoms of Pt at an early stage of the Pt growth when the Pt loading is very low on the substrate. For example, an Au@Pt core-shell structure showed excellent FAOR activity only when the number of the Pt layers on the Au substrate was <0.1, i.e., the coverage of Pt on the Au substrate was <10%. [18] Unfortunately, the substrates for the growth of Pt are usually noble metals as well, e.g., Au, to avoid any galvanic replacement reaction in the synthesis and oxidative etching in the electrocatalysis. The sparse dispersion of Pt on these noble metal substrates significantly increases the cost of the catalysts and impedes their wide applications.There have been electrochemical methods that can control the ensemble size of noble metals such as Pt on foreign substrates by taking advantage of the underpotential deposition (UPD) phenomenon. [19][20][21][22][23][24] Metal atoms such as Cu and Pb form a full atomic layer on a noble metal substrate, due to the UPD, which are then substituted by Pt through the galvanic replacement reaction, leading to the formation of a (sub-)monolayer Pt atoms on the noble metal substrate. [19][20][21][22] Another approach utilizes the UPD of H to achieve the self-terminating growth of Decreasing the ensemble size of Pt to isolated single atoms is the key to enhance the electrocatalytic formic acid oxidation reaction (FAOR) by bypassing the indirect reaction path that involves the poisoning by the CO intermediate. However, it is challenging to construct isolated Pt single atoms on a foreign metal substrate, especially at high Pt loadings, because Pt tends to form large ensembles due to the high Pt-Pt bond energy. Herein, a ligandmediated self-terminating growth strategy is reported for reliably controlling the ensemble size of Pt on an Au substrate. The key is to introduce a ligan...

show abstract

Trace Pd modified intermetallic PtBi nanoplates towards efficient formic acid electrocatalysis

Abstract: Promoting formic acid electrochemical oxidation through the dehydrogenation path is critical for the development of direct liquid fuel cells. Herein, we report the modification of intermetallic PtBi hexagonal nanoplates by...

Cited by 41 publications

References 50 publications

Hexagonal PtBi Intermetallic Inlaid with Sub‐Monolayer Pb Oxyhydroxide Boosts Methanol Oxidation

Hexagonal PtBi Intermetallic Inlaid with Sub‐Monolayer Pb Oxyhydroxide Boosts Methanol Oxidation

Recent Progress on Structurally Ordered Materials for Electrocatalysis

Ligand‐Mediated Self‐Terminating Growth of Single‐Atom Pt on Au Nanocrystals for Improved Formic Acid Oxidation Activity

Contact Info

Product

Resources

About