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Cited by 193Electrocatalysts for Energy ConversionFuel Cells and Related MaterialsCatalytic Processes in Materials Science

The DOI matches its Crossref record; 55 of the 55 references it cites were found in a registry or an index.

Small molecule-assisted synthesis of carbon supported platinum intermetallic fuel cell catalysts

Open access
Song, Tian-Wei, Xu, Cong, Sheng, Zhu-Tao, Yan, Hui-Kun, Tong, Lei, Liu, Jun, Zeng, Wei-Jie, Zuo, Lu-Jie, Yin, Peng, Zuo, Ming, Chu, Sheng-Qi, Chen, Ping, Liang, Hai-Wei·2022·Nature Communications
DOI 10.1038/s41467-022-34037-7PMC PMC9622856
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Abstract

Supported ordered intermetallic compounds exhibit superior catalytic performance over their disordered alloy counterparts in diverse reactions. But the synthesis of intermetallic compounds catalysts often requires high-temperature annealing that leads to the sintering of metals into larger crystallites. Herein, we report a small molecule-assisted impregnation approach to realize the general synthesis of a family of intermetallic catalysts, consisting of 18 binary platinum intermetallic compounds supported on carbon blacks. The molecular additives containing heteroatoms (that is, O, N, or S) can be coordinated with platinum in impregnation and thermally converted into heteroatom-doped graphene layers in high-temperature annealing, which significantly suppress alloy sintering and insure the formation of small-sized intermetallic catalysts. The prepared optimal PtCo intermetallics as cathodic oxygen-reduction catalysts exhibit a high mass activity of 1.08 A mg Pt–1 at 0.9 V in H 2-O 2 fuel cells and a rated power density of 1.17 W cm–2 in H 2-air fuel cells.

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Fig. 1 Screening small molecules for suppressing metal sintering. a The structures of the molecules used as additives for suppressing metal sintering. b XRD (solid shadow column) and STEM (twill stripes column) sizes of PtCo particles with various molecule additives used for the catalyst synthesis at 700 °C. STEM statistics of particle size distribution of PtCo synthesized without (c) and with three representative molecule additives, including SAc (d), DCDA (e), and STG (f).
Fig. 1 Screening small molecules for suppressing metal sintering. a The structures of the molecules used as additives for suppressing metal sintering. b XRD (solid shadow column) and STEM (twill stripes column) sizes of PtCo particles with various molecule additives used for the catalyst synthesis at 700 °C. STEM statistics of particle size distribution of PtCo synthesized without (c) and with three representative molecule additives, including SAc (d), DCDA (e), and STG (f).CC BY · PubMed Central
Fig. 2 STG-assisted synthesis of Pt-IMCs catalyst libraries. a Periodic table showing Pt (highlighted in red) and base metal elements (highlighted in yellow) that constitute Pt-IMCs catalysts libraries. Comparison of the XRD patterns of PtFe (b), PtCo (c), and PtNi (d) prepared with and without STG. e Comparison of XRD particle size of the 18 Pt-IMCs catalysts prepared with and without STG.
Fig. 2 STG-assisted synthesis of Pt-IMCs catalyst libraries. a Periodic table showing Pt (highlighted in red) and base metal elements (highlighted in yellow) that constitute Pt-IMCs catalysts libraries. Comparison of the XRD patterns of PtFe (b), PtCo (c), and PtNi (d) prepared with and without STG. e Comparison of XRD particle size of the 18 Pt-IMCs catalysts prepared with and without STG.CC BY · PubMed Central
Fig. 3 Structural characterization of the Pt-IMCs catalysts. HAADF-STEM images of PtFe (a), PtCo (b), and PtNi (c) prepared with STG. Inserts were the corresponding statistics of particle size distribution. EDS elemental mapping of PtFe (d), PtCo (e), and PtNi (f) prepared with STG.
Fig. 3 Structural characterization of the Pt-IMCs catalysts. HAADF-STEM images of PtFe (a), PtCo (b), and PtNi (c) prepared with STG. Inserts were the corresponding statistics of particle size distribution. EDS elemental mapping of PtFe (d), PtCo (e), and PtNi (f) prepared with STG.CC BY · PubMed Central
Fig. 4 Atomic scale HAADF-STEM characterization of Pt-IMCs. Atomic-resolution HAADF-STEM images and alternative intensity profiles of PtCo (a), Pt3Co (b), and PtCu (c). The alternative intensity profiles were obtained from the corresponding region marked by red dashed rectangle.
Fig. 4 Atomic scale HAADF-STEM characterization of Pt-IMCs. Atomic-resolution HAADF-STEM images and alternative intensity profiles of PtCo (a), Pt3Co (b), and PtCu (c). The alternative intensity profiles were obtained from the corresponding region marked by red dashed rectangle.CC BY · PubMed Central
Fig. 5 Anti-sintering mechanism. a UV–Vis spectra of the H2PtCl6·6H2O solution, STG solution, the H2PtCl6·6H2O/STG solution, and the H2PtCl6·6H2O/SAc solution. XPS results of the Pt 4f (b) and Co 2p (c) orbits of the STG-PtCo/C precursor powder and PtCo/C precursor powder. d TG result of STG-PtCo/C raw powder from room temperature to 900 °C. e MS signal of CH2-SH fragment obtained from the STG/C powder and STG-PtCo/C precursor powder. f R space of the XAFS results of the standard PtS2, and PtCo IMCs catalysts prepared with and without STG. g Proposed anti-sintering mechanism of the STG-assisted method.
Fig. 5 Anti-sintering mechanism. a UV–Vis spectra of the H2PtCl6·6H2O solution, STG solution, the H2PtCl6·6H2O/STG solution, and the H2PtCl6·6H2O/SAc solution. XPS results of the Pt 4f (b) and Co 2p (c) orbits of the STG-PtCo/C precursor powder and PtCo/C precursor powder. d TG result of STG-PtCo/C raw powder from room temperature to 900 °C. e MS signal of CH2-SH fragment obtained from the STG/C powder and STG-PtCo/C precursor powder. f R space of the XAFS results of the standard PtS2, and PtCo IMCs catalysts prepared with and without STG. g Proposed anti-sintering mechanism of the STG-assisted method.CC BY · PubMed Central
Fig. 6 Electrocatalytic performance. RDE mass activity (a), and specific activity (b) of the STG-assisted Pt-IMCs catalysts and TKK-30 wt% Pt/C. The Pt loading in RDE tests were in the range of 11~13 µg cm–2. c Correlation between specific activity and calculated surface strain of the five L10 PtM catalysts and Pt/C. The error bars in a, b, and c were obtained after three parallel experiments. d Mass activity loss of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700 after 30,000 cycles’ ADT. e H2-air polarization curves and power density plots of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700. For all MEA, the cathode and anode loadings were controlled to be 0.1 and 0.025 mgPt cm–2, respectively. Test conditions: 80 °C, 100% RH, 150 kPaabs, outlet H2-air at high stoichiometries (H2 and air flow rates were fixed at 0.5 and 2.0 L min–1, respectively). f Voltage loss at 0.8 A cm–2 of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700 after 30,000 cycles’ ADT.
Fig. 6 Electrocatalytic performance. RDE mass activity (a), and specific activity (b) of the STG-assisted Pt-IMCs catalysts and TKK-30 wt% Pt/C. The Pt loading in RDE tests were in the range of 11~13 µg cm–2. c Correlation between specific activity and calculated surface strain of the five L10 PtM catalysts and Pt/C. The error bars in a, b, and c were obtained after three parallel experiments. d Mass activity loss of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700 after 30,000 cycles’ ADT. e H2-air polarization curves and power density plots of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700. For all MEA, the cathode and anode loadings were controlled to be 0.1 and 0.025 mgPt cm–2, respectively. Test conditions: 80 °C, 100% RH, 150 kPaabs, outlet H2-air at high stoichiometries (H2 and air flow rates were fixed at 0.5 and 2.0 L min–1, respectively). f Voltage loss at 0.8 A cm–2 of the MEAs made with cathode catalysts of STG-assisted PtCo, Umic-30 wt% PtCo, TKK-30 wt% Pt/C, and TKK-30 wt% Pt/C-700 after 30,000 cycles’ ADT.CC BY · PubMed Central

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Metadata

Authors
Song, T.-W., Xu, C., Sheng, Z.-T., Yan, H.-K., Tong, L., Liu, J., Zeng, W.-J., Zuo, L.-J., Yin, P., Zuo, M., Chu, S.-Q., Chen, P., & Liang, H.-W.
Affiliations
  • University of Science and Technology of China (CN)
  • Anhui Normal University (CN)
  • Chinese Academy of Sciences (CN)
  • Anhui University (CN)
Corresponding author
Liang, Hai-Wei
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2022-10-31
Volume
13
Issue
1
Pages
6521-6521
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-022-34037-7
PMC
PMC9622856
OpenAlex
W4307897536
Cited by
193
References
55
Citations by year
2026: 40 · 2025: 64 · 2024: 53 · 2023: 36
FWCI
6.89
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • National Natural Science Foundation of China (22071225 and 51971211)
  • Youth Innovation Promotion Association of the Chinese Academy of Sciences (2017483)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
Keywords
carbon-supported catalysts, heteroatom-doped graphene, sintering suppression, high-temperature annealing, oxygen reduction reaction, fuel cell catalysts, H2/O2 fuel cells, H2/air fuel cells, mass activity

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