Core–Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction
Open accessAbstract
The development of core–shell structures remains a fundamental challenge for pure metallic aerogels. Here we report the synthesis of PdxAu‐Pt core–shell aerogels composed of an ultrathin Pt shell and a composition‐tunable PdxAu alloy core. The universality of this strategy ensures the extension of core compositions to Pd transition‐metal alloys. The core–shell aerogels exhibited largely improved Pt utilization efficiencies for the oxygen reduction reaction and their activities show a volcano‐type relationship as a function of the lattice parameter of the core substrate. The maximum mass and specific activities are 5.25 A mg Pt−1 and 2.53 mA cm−2, which are 18.7 and 4.1 times higher than those of Pt/C, respectively, demonstrating the superiority of the core–shell metallic aerogels. The proposed core‐based activity descriptor provides a new possible strategy for the design of future core–shell electrocatalysts.
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
Only the Pd-Pt, Pt-Ni, and PdxAu-Pt core-shell aerogels have been reported to date.
“only the Pd–Pt, Pt–Ni, and PdxAu-Pt core–shell aerogels have been reported to date.[15,16,40]”
From Engineering Multimetallic Aerogels for pH‐Universal HER and ORR Electrocatalysis (2020) · cites this paper as [15]
The paper reports PdₓAu–Pt and Pd–Ni–Pt core–shell aerogels, but it also says it fabricated Pd₃Co–Pt and Pd₃Cu–Pt core–shell aerogels (main text, page unavailable; Figure S14). Those additional examples contradict the claim that only the three listed types had been reported. (LLM, conf=0.88)
Checked by a reasoning model — may be wrong.
Experimental — accuracy not yet measuredThe preparation process of NMAs is costly and time-consuming, requiring a high concentration of precursors, a complicated procedure, and yielding uneven size of ligaments.
“the preparation process of NMAs is costly and time-consuming, in addition to requirement of high concentration of precursors, complicated procedure, and uneven size of ligaments of NMAs.”
From Ultrafast Generation of Nanostructured Noble Metal Aerogels by a Microwave Method for Electrocatalytic Hydrogen Evolution and Ethanol Oxidation (2021) · cites this paper as [21]
The Additional information section reports hydrogel gelation times of one to five days, supporting the time-consuming aspect. It describes a “facile” preparation using 0.2 mM precursors, rather than a complicated procedure requiring high precursor concentrations. The cited passages do not establish that preparation is costly or that ligament sizes are uneven; page numbers are unavailable in our copy. (LLM, conf=0.85)
Experimental — accuracy not yet measuredThe lower stability of Pt/C might be attributed to the delamination of supported carbon during operation, while the self-supported Au-Pt aerogel does not have such issues.
“The lower stability of Pt/C might be attributed to the delamination of supported carbon during operation, while the self-supported Au–Pt aerogel does not have such issues, as reported for the Pt–Pd and in Pt–Ni aerogels.[15,16]”
From Engineering Multimetallic Aerogels for pH‐Universal HER and ORR Electrocatalysis (2020) · cites this paper as [15]
The stability results (section labeled Abstract; page unavailable) report less mass-activity loss for a Pd20Au–Pt aerogel than for Pt/C after 10,000 cycles, and say the aerogel retained its network structure. The paper does not attribute Pt/C’s loss to carbon-support delamination; it discusses particle aggregation instead. Its tested aerogel is Pd–Au–Pt, not simply Au–Pt. (LLM, conf=0.85)
Experimental — accuracy not yet measuredUnsupported trimetallic PdAuPt aerogel shows excellent performance toward the oxygen reduction reaction (ORR), outperforming state-of-the-art Pt/C catalysts.
“unsupported trimetallic PdAuPt aerogel has been reported to show an excellent performance toward the oxygen reduction reaction (ORR), also outperforming the state-of-the-art Pt/C catalysts [36].”
From Partially oxidized ruthenium aerogel as highly active bifunctional electrocatalyst for overall water splitting in both alkaline and acidic media (2022) · cites this paper as [36]
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
The citation lists haven’t been fetched yet
References 39 · Cited by 185
Research works printed but not linked: 56
- V. R. Stamenkovic, D. Strmcnik, P. P. Lopes, N. M. Markovic, Nat. Mater. 2016, 16, 57-69;
- S. Chu, Y. Cui, N. Liu, Nat. Mater. 2016, 16, 16-22.
- M. K. Debe, Nature 2012, 486, 43-51.
- X. Q. Huang, Z. P. Zhao, L. Cao, Y. Chen, E. B. Zhu, Z. Y. Lin, M. F. Li, A. M. Yan, A. Zettl, Y. M. Wang, X. F. Duan, T. Mueller, Y. Huang, Science 2015, 348, 1230-1234;
- L. Zhang, L. T. Roling, X. Wang, M. Vara, M. Chi, J. Liu, S. I. Choi, J. Park, J. A. Herron, Z. Xie, M. Mavrikakis, Y. Xia, Science 2015, 349, 412-416;
- L. Bu, N. Zhang, S. Guo, X. Zhang, J. Li, J. Yao, T. Wu, G. Lu, J. Y. Ma, D. Su, X. Huang, Science 2016, 354, 1410-1414.
- Z. L. Wang, D. Xu, H. X. Zhong, J. Wang, F. L. Meng, X. B. Zhang, Sci. Adv. 2015, 1, e1400035;
- H.-x. Zhong, K. Li, Q. Zhang, J. Wang, F.-l. Meng, Z.-j. Wu, J.-m. Yan, X.-b. Zhang, NPG Asia Mater. 2016, 8, e308;
- W. J. Jiang, L. Gu, L. Li, Y. Zhang, X. Zhang, L. J. Zhang, J. Q. Wang, J. S. Hu, Z. Wei, L. J. Wan, J. Am. Chem. Soc. 2016, 138, 3570- 3578;
- H. X. Zhong, J. Wang, Y. W. Zhang, W. L. Xu, W. Xing, D. Xu, Y. F. Zhang, X. B. Zhang, Angew. Chem. Int. Ed. 2014, 53, 14235- 14239;
- F. L. Meng, Z. L. Wang, H. X. Zhong, J. Wang, J. M. Yan, X. B. Zhang, Adv. Mater. 2016, 28, 7948-7955.
- Y. J. Kang, P. D. Yang, N. M. Markovic, V. R. Stamenkovic, Nano Today 2016, 11, 587-600;
- H. Mistry, A. S. Varela, S. Kühl, P. Strasser, B. R. Cuenya, Nat. Rev. Mater. 2016, 1, 16009.
- D. F. van der Vliet, C. Wang, D. Tripkovic, D. Strmcnik, X. F. Zhang, M. K. Debe, R. T. Atanasoski, N. M. Markovic, V. R. Stamenkovic, Nat. Mater. 2012, 11, 1051-1058;
- B. Cai, S. Henning, J. Herranz, T. J. Schmidt, A. Eychmüller, Adv. Energy Mater. 2017, 7, 1700548.
- W. Liu, A. K. Herrmann, N. C. Bigall, P. Rodriguez, D. Wen, M. Oezaslan, T. J. Schmidt, N. Gaponik, A. Eychmüller, Acc. Chem. Res. 2015, 48, 154-162.
- B. Cai, D. Wen, W. Liu, A. K. Herrmann, A. Benad, A. Eychmüller, Angew. Chem. Int. Ed. 2015, 54, 13101-13105;
- B. Cai, A. Dianat, R. Hubner, W. Liu, D. Wen, A. Benad, L. Sonntag, T. Gemming, G. Cuniberti, A. Eychmüller, Adv. Mater. 2017, 29, 1605254.
- W. Liu, P. Rodriguez, L. Borchardt, A. Foelske, J. Yuan, A. K. Herrmann, D. Geiger, Z. Zheng, S. Kaskel, N. Gaponik, R. Kotz, T. J. Schmidt, A. Eychmüller, Angew. Chem. Int. Ed. 2013, 52, 9849-9852;
- D. Wen, A. K. Herrmann, L. Borchardt, F. Simon, W. Liu, S. Kaskel, A. Eychmüller, J. Am. Chem. Soc. 2014, 136, 2727-2730.
- S. Guo, S. Zhang, S. Sun, Angew. Chem. Int. Ed. 2013, 52, 8526- 8544;
- M. Shao, Q. Chang, J. P. Dodelet, R. Chenitz, Chem. Rev. 2016, 116, 3594-3657.
- Q. R. Shi, C. Z. Zhu, Y. J. Li, H. B. Xia, M. H. Engelhard, S. F. Fu, D. Du, Y. H. Lin, Chem. Mater. 2016, 28, 7928-7934.
- X. Wang, S. I. Choi, L. T. Roling, M. Luo, C. Ma, L. Zhang, M. Chi, J. Liu, Z. Xie, J. A. Herron, M. Mavrikakis, Y. Xia, Nat. Comm. 2015, 6, 7594.
- C. Zhu, D. Du, A. Eychmüller, Y. Lin, Chem. Rev. 2015, 115, 8896- 8943.
- X. Tian, J. Luo, H. Nan, H. Zou, R. Chen, T. Shu, X. Li, Y. Li, H. Song, S. Liao, R. R. Adzic, J. Am. Chem. Soc. 2016, 138, 1575-1583;
- K. Sasaki, H. Naohara, Y. Choi, Y. Cai, W. F. Chen, P. Liu, R. R. Adzic, Nat. Comm. 2012, 3, 1115.
- H. H. Li, S. Y. Ma, Q. Q. Fu, X. J. Liu, L. Wu, S. H. Yu, J. Am. Chem. Soc. 2015, 137, 7862-7868.
- J. Hu, L. Wu, K. A. Kuttiyiel, K. R. Goodman, C. Zhang, Y. Zhu, M. B. Vukmirovic, M. G. White, K. Sasaki, R. R. Adzic, J. Am. Chem. Soc. 2016, 138, 9294-9300.
- Y. C. Xing, Y. Cai, M. B. Vukmirovic, W. P. Zhou, H. Karan, J. X. Wang, R. R. Adzic, J. Phys. Chem. Lett. 2010, 1, 3238-3242.
- M. Escudero-Escribano, P. Malacrida, M. H. Hansen, U. G. Vej-Hansen, A. Velazquez-Palenzuela, V. Tripkovic, J. Schiotz, J. Rossmeisl, I. E. Stephens, I. Chorkendorff, Science 2016, 352, 73-76.
- M. Du, L. Cui, Y. Cao, A. J. Bard, J. Am. Chem. Soc. 2015, 137, 7397-7403;
- H. Wang, S. Xu, C. Tsai, Y. Li, C. Liu, J. Zhao, Y. Liu, H. Yuan, F. Abild-Pedersen, F. B. Prinz, J. K. Norskov, Y. Cui, Science 2016, 354, 1031-1036.
- F. Calle-Vallejo, M. T. Koper, A. S. Bandarenka, Chem. Soc. Rev. 2013, 42, 5210-5230. References
- Brankovic, S. R.; Wang, J. X.; Adzic, R. R. Surface Science 2001, 474, L173.
- Adzic, R. R.; Zhang, J.; Sasaki, K.; Vukmirovic, M. B.; Shao, M.; Wang, J. X.; Nilekar, A. U.; Mavrikakis, M.; Valerio, J. A.; Uribe, F. Topics in Catalysis 2007, 46, 249.
- Vukmirovic, M. B.; Bliznakov, S. T.; Sasaki, K.; Wang, J. X.; Adzic, R. R. Electrochem. Soc. Interface 2011, 20, 33.
- Sasaki, K.; Marinkovic, N.; Isaacs, H. S.; Adzic, R. R. ACS Catal. 2016, 6, 69-76.
- Ravel, B., Newville, M. Synchrotron Radiation 2005, 12, 537.
- Sasaki, K.; Wang, J. X.; Naohara, H.; Marinkovic, N.; More, K.; Inada, H.; Adzic, R. R. Electrochimica Acta 2010, 55, 2645.
- Menard, L. D.; Wang, Q.; Kang, J. H.; Sealey, A. J.; Girolami, G. S.; Teng, X.; Frenkel, A. I.; Nuzzo, R. G. Physical Review B 2009, 80, 064111.
- Frenkel, A. Zeitschrift Fur Kristallographie 2007, 222, 605.
- Liu, W.; Herrmann, A. K.; Bigall, N. C.; Rodriguez, P.; Wen, D.; Oezaslan, M.; Schmidt, T. J.; Gaponik, N.; Eychmüller, A. Acc. Chem. Res. 2015, 48, 154.
- Zhu, C.; Du, D.; Eychmüller, A.; Lin, Y. Chem. Rev. 2015, 115, 8896.
- Wang, X.; Choi, S. I.; Roling, L. T.; Luo, M.; Ma, C.; Zhang, L.; Chi, M.; Liu, J.; Xie, Z.; Herron, J. A.; Mavrikakis, M.; Xia, Y. Nat. Comm. 2015, 6, 7594.
- Li, H. H.; Ma, S. Y.; Fu, Q. Q.; Liu, X. J.; Wu, L.; Yu, S. H. J. Am. Chem. Soc. 2015, 137, 7862.
- Zhang, S.; Hao, Y.; Su, D.; Doan-Nguyen, V. V.; Wu, Y.; Li, J.; Sun, S.; Murray, C. B. J. Am. Chem. Soc. 2014, 136, 15921.
- Zhao, X.; Chen, S.; Fang, Z.; Ding, J.; Sang, W.; Wang, Y.; Zhao, J.; Peng, Z.; Zeng, J. J. Am. Chem. Soc. 2015, 137, 2804.
- Wang, X.; Vara, M.; Luo, M.; Huang, H.; Ruditskiy, A.; Park, J.; Bao, S.; Liu, J.; Howe, J.; Chi, M.; Xie, Z.; Xia, Y. J. Am. Chem. Soc. 2015, 137, 15036.
- Tian, X.; Luo, J.; Nan, H.; Zou, H.; Chen, R.; Shu, T.; Li, X.; Li, Y.; Song, H.; Liao, S.; Adzic, R. R. J. Am. Chem. Soc. 2016, 138, 1575.
- Hu, J.; Wu, L.; Kuttiyiel, K. A.; Goodman, K. R.; Zhang, C.; Zhu, Y.; Vukmirovic, M. B.; White, M. G.; Sasaki, K.; Adzic, R. R. J. Am. Chem. Soc. 2016, 138, 9294.
- Choi, S. I.; Shao, M.; Lu, N.; Ruditskiy, A.; Peng, H. C.; Park, J.; Guerrero, S.; Wang, J.; Kim, M. J.; Xia, Y. ACS Nano 2014, 8, 10363.
- Bu, L.; Zhang, N.; Guo, S.; Zhang, X.; Li, J.; Yao, J.; Wu, T.; Lu, G.; Ma, J. Y.; Su, D.; Huang, X. Science 2016, 354, 1410.
- Chen, C.; Kang, Y.; Huo, Z.; Zhu, Z.; Huang, W.; Xin, H. L.; Snyder, J. D.; Li, D.; Herron, J. A.; Mavrikakis, M.; Chi, M.; More, K. L.; Li, Y.; Markovic, N. M.; Somorjai, G. A.; Yang, P.; Stamenkovic, V. R. Science 2014, 343, 1339.
- Huang, X. Q.; Zhao, Z. P.; Cao, L.; Chen, Y.; Zhu, E. B.; Lin, Z. Y.; Li, M. F.; Yan, A. M.; Zettl, A.; Wang, Y. M.; Duan, X. F.; Mueller, T.; Huang, Y. Science 2015, 348, 1230.
- Li, M.; Zhao, Z.; Cheng, T.; Fortunelli, A.; Chen, C. Y.; Yu, R.; Zhang, Q.; Gu, L.; Merinov, B. V.; Lin, Z.; Zhu, E.; Yu, T.; Jia, Q.; Guo, J.; Zhang, L.; Goddard, W. A., 3rd; Huang, Y.; Duan, X. Science 2016, 354, 1414.
- Authors
- Cai, B., Hübner, R., Sasaki, K., Zhang, Y., Su, D., Ziegler, C., Vukmirovic, M. B., Rellinghaus, B., Adzic, R. R., & Eychmüller, A.
- Affiliations
- Brookhaven National Laboratory (US)
- Helmholtz-Zentrum Dresden-Rossendorf (DE)
- Technische Universität Dresden (DE)
- Leibniz Institute for Solid State and Materials Research (DE)
- Chemistry Division and Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
- Corresponding author
- Eychmüller, Alexander
- ORCID
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2018-02-08
- Volume
- 57
- Issue
- 11
- Pages
- 2963-2966
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W2790566095
- Cited by
- 185
- References
- 39
- Citations by year
- 2026: 10 · 2025: 12 · 2024: 11 · 2023: 22 · 2022: 21 · 2021: 26 · 2020: 35 · 2019: 29 · 2018: 19
- FWCI
- 6.08
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Licence
- Locations
- Angewandte Chemie International Edition (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Qucosa (Saxon State and University Library Dresden) (submittedVersion, other-oa)
- Funders
- U.S. Department of Energy (DE-SC0012704)
- Deutsche Forschungsgemeinschaft (ZuK support the best)
- FP7 Ideas: European Research Council (AdG AEROCAT)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- platinum utilization, oxygen reduction reaction, Au-Pd alloys, lattice parameters, electrocatalysts, mass and specific activity
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review