Breaking Ordered Atomic Arrangement into Disordered Amorphous Structure for High Electrocatalytic Performance

Abstract

Noble metal-based intermetallic compounds (IMCs) with ordered atomic arrangements exhibit remarkable electrocatalytic activity owing to their unique crystal and electronic structures. During the past years, great advance has been made in the development of noble metal-based IMCs. Recently, Lu and coworkers reported ultrathin “amorphous/intermetallic” (A/IMC) heterophase PtPbBi nanosheets (NSs) with a thickness of 2.5 ± 0.3 nm. The oxidative etching effect caused by the coexistence of O₂ and Br^‒ ions plays a crucial role in the formation of the IMC and unique two-dimensional structure with irregular shapes and curled edges. This study shows that fabricating an A/IMC heterophase structure with a multimetallic composition can effectively enhance the catalytic performances of noble metal-based electrocatalysts.

References

[1] YinK, ChaoY, LvF, et al. . One nanometer PtIr nanowires as high-efficiency bifunctional catalysts for electrosynthesis of ethanol into high value-added multicarbon compound coupled with hydrogen production. J Am Chem Soc, 2021, 143(29): 10822-10827

[2] YangG, ZhangQ, YuH, et al. . Platinum-based ternary catalysts for the electrooxidation of ethanol. Particuology, 2021, 58: 169-186

[3] GuoY, YangX, LiuX, et al. . Coupling methanol oxidation with hydrogen evolution on bifunctional Co-doped Rh electrocatalyst for efficient hydrogen generation. Adv Funct Materials, 2023, 33(2): 2209134

[4] HeC, MaC, XiaJ, et al. . Low-iridium-content IrIn₂ intermetallics with an unconventional face-centered orthorhombic phase for efficient overall water splitting. Adv Funct Materials, 2024, 34(8): 2311683

[5] HanS, SunH, MaC, et al. . Wet-chemical epitaxial growth of metastable-phase intermetallic electrocatalysts. Adv Funct Mater, 2024, 34: 2403023

[6] LiJ, SunS. Intermetallic nanoparticles: synthetic control and their enhanced electrocatalysis. Acc Chem Res, 2019, 52(7): 2015-2025

[7] MaC, ZhangH, XiaJ, et al. . Screening of intermetallic compounds based on intermediate adsorption equilibrium for electrocatalytic nitrate reduction to ammonia. J Am Chem Soc, 2024, 146(29): 20069-20079

[8] MaX, MaC, XiaJ, et al. . Heterophase intermetallic compounds for electrocatalytic hydrogen production at industrial-scale current densities. J Am Chem Soc, 2024, 146(30): 20594-20603

[9] YanY, DuJS, GilroyKD, et al. . Intermetallic nanocrystals: syntheses and catalytic applications. Adv Mater, 2017, 29(14): 1605997

[10] RößnerL, ArmbrüsterM. Electrochemical energy conversion on intermetallic compounds: a review. ACS Catal, 2019, 9(3): 2018-2062

[11] JiangG, HanD, HanZ, et al. . Rational manipulation of intermediates on copper for CO₂ electroreduction toward multicarbon products. Trans Tianjin Univ, 2022, 28(4): 265-291

[12] HuangY, HeC, ChengC, et al. . Pulsed electroreduction of low-concentration nitrate to ammonia. Nat Commun, 2023, 14: 7368

[13] YunQ, LuQ, LiC, et al. . Synthesis of PdM (M = Zn, Cd, ZnCd) nanosheets with an unconventional face-centered tetragonal phase as highly efficient electrocatalysts for ethanol oxidation. ACS Nano, 2019, 13(12): 14329-14336

[14] ChenW, LuoS, SunM, et al. . High-entropy intermetallic PtRhBiSnSb nanoplates for highly efficient alcohol oxidation electrocatalysis. Adv Mater, 2022, 34(43) e2206276

[15] ZhangH, LiY, ChengC, et al. . Isolated electron-rich ruthenium atoms in intermetallic compounds for boosting electrochemical nitric oxide reduction to ammonia. Angew Chem Int Ed Engl, 2023, 62(4) e202213351

[16] LingT, WangJJ, ZhangH, et al. . Freestanding ultrathin metallic nanosheets: materials, synthesis, and applications. Adv Mater, 2015, 27(36): 5396-5402

[17] FanJ, YuS, QiK, et al. . Synthesis of ultrathin wrinkle-free PdCu alloy nanosheets for modulating d-band electrons for efficient methanol oxidation. J Mater Chem A, 2018, 6(18): 8531-8536

[18] HanA, ZhangZ, LiX, et al. . Atomic thickness catalysts: synthesis and applications. Small Meth, 2020, 4(9): 2000248

[19] LiW, ZhaoY, LiuY, et al. . Exploiting Ru-induced lattice strain in CoRu nanoalloys for robust bifunctional hydrogen production. Angew Chem Int Ed Engl, 2021, 60(6): 3290-3298

[20] YunQ, GeY, ShiZ, et al. . Recent progress on phase engineering of nanomaterials. Chem Rev, 2023, 123(23): 13489-13692

[21] FengF, MaC, HanS, et al. . Breaking highly ordered PtPbBi intermetallic with disordered amorphous phase for boosting electrocatalytic hydrogen evolution and alcohol oxidation. Angew Chem Int Ed Engl, 2024, 63(25) e202405173

RIGHTS & PERMISSIONS

The Author(s) under exclusive licence to Tianjin University