In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

Guowei Li; Seunghyun Khim; Celesta S. Chang; Chenguang Fu; Nabhanila Nandi; Fan Li; Qun Yang; Graeme R. Blake; Stuart Parkin; Gudrun Auffermann; Yan Sun; David A. Muller; Andrew P. Mackenzie; Claudia Felser

doi:10.1021/acsenergylett.9b01527

In situ modification of delafossite-type PdCoO₂ bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

Guowei Li, Seunghyun Khim, Celesta S. Chang, Chenguang Fu, Nabhanila Nandi, Fan Li, Qun Yang, Graeme R. Blake, Stuart Parkin, Gudrun Auffermann, Yan Sun, David A. Muller, Andrew P. Mackenzie, Claudia Felser

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Abstract

The observation of extraordinarily high conductivity in delafossite-type PdCoO₂ is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO₂. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO₂ as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm^-2, accompanied by excellent long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit excellent hydrogen sorption/desorption reversibility, creating more active sites for hydrogen access. The bulk PdCoO₂ single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer.

Original language	English
Pages (from-to)	2185-2191
Number of pages	7
Journal	ACS Energy Letters
Volume	4
Issue number	9
Early online date	15 Aug 2019
DOIs	https://doi.org/10.1021/acsenergylett.9b01527
Publication status	Published - 13 Sept 2019

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Copyright © 2019 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
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In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution (dataset)
Li, G. (Creator), Khim, S. (Creator), Chang, C. (Creator), Fu, C. (Creator), Nandi, N. (Creator), Li, F. (Creator), Yang, Q. (Creator), Blake, G. (Creator), Parkin, S. (Creator), Auffermann, G. (Creator), Sun, Y. (Creator), Muller, D. (Creator), Mackenzie, A. P. (Creator) & Felser, C. (Creator), University of St Andrews, 28 Aug 2019
DOI: 10.17630/4f818aaa-e937-46e6-9257-161689cdf399
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Li, G., Khim, S., Chang, C. S., Fu, C., Nandi, N., Li, F., Yang, Q., Blake, G. R., Parkin, S., Auffermann, G., Sun, Y., Muller, D. A., Mackenzie, A. P., & Felser, C. (2019). In situ modification of delafossite-type PdCoO₂ bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution. ACS Energy Letters, 4(9), 2185-2191. https://doi.org/10.1021/acsenergylett.9b01527

@article{7679730d293d4874943eefdb2067da92,

title = "In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution",

abstract = "The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm-2, accompanied by excellent long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit excellent hydrogen sorption/desorption reversibility, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer. ",

author = "Guowei Li and Seunghyun Khim and Chang, {Celesta S.} and Chenguang Fu and Nabhanila Nandi and Fan Li and Qun Yang and Blake, {Graeme R.} and Stuart Parkin and Gudrun Auffermann and Yan Sun and Muller, {David A.} and Mackenzie, {Andrew P.} and Claudia Felser",

note = "This work was financially supported by the European Research Council (ERC Advanced Grant No. 291472 'Idea Heusler') and ERC Advanced Grant (No. 742068). TOPMAT{\textquoteright}. Electron Microscopy (C.C., D.M.) supported by the U.S. Department of Energy, Basic Energy Sciences grant No. DE-SC0019445, with facility support from the National Science Foundation NSF Grant No. DMR-1719875.",

year = "2019",

month = sep,

day = "13",

doi = "10.1021/acsenergylett.9b01527",

language = "English",

volume = "4",

pages = "2185--2191",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "American Chemical Society (ACS)",

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Li, G, Khim, S, Chang, CS, Fu, C, Nandi, N, Li, F, Yang, Q, Blake, GR, Parkin, S, Auffermann, G, Sun, Y, Muller, DA, Mackenzie, AP & Felser, C 2019, 'In situ modification of delafossite-type PdCoO₂ bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution', ACS Energy Letters, vol. 4, no. 9, pp. 2185-2191. https://doi.org/10.1021/acsenergylett.9b01527

TY - JOUR

T1 - In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

AU - Li, Guowei

AU - Khim, Seunghyun

AU - Chang, Celesta S.

AU - Fu, Chenguang

AU - Nandi, Nabhanila

AU - Li, Fan

AU - Yang, Qun

AU - Blake, Graeme R.

AU - Parkin, Stuart

AU - Auffermann, Gudrun

AU - Sun, Yan

AU - Muller, David A.

AU - Mackenzie, Andrew P.

AU - Felser, Claudia

N1 - This work was financially supported by the European Research Council (ERC Advanced Grant No. 291472 'Idea Heusler') and ERC Advanced Grant (No. 742068). TOPMAT’. Electron Microscopy (C.C., D.M.) supported by the U.S. Department of Energy, Basic Energy Sciences grant No. DE-SC0019445, with facility support from the National Science Foundation NSF Grant No. DMR-1719875.

PY - 2019/9/13

Y1 - 2019/9/13

N2 - The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm-2, accompanied by excellent long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit excellent hydrogen sorption/desorption reversibility, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer.

AB - The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm-2, accompanied by excellent long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit excellent hydrogen sorption/desorption reversibility, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer.

U2 - 10.1021/acsenergylett.9b01527

DO - 10.1021/acsenergylett.9b01527

M3 - Article

SN - 2380-8195

VL - 4

SP - 2185

EP - 2191

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 9

ER -

In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

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In situ modification of delafossite-type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution (dataset)

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In situ modification of delafossite-type PdCoO₂ bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution