Modular Iron–Bipyridine-Based Conjugated Aerogels as Catalysts for Oxygen Reduction Reaction

Peles-Strahl, Leigh; Honig, Hilah C.; Persky, Yeela; Cullen, David A.; Dahan, Adi; Elbaz, Lior

doi:10.1021/acscatal.3c03998

Title: Modular Iron–Bipyridine-Based Conjugated Aerogels as Catalysts for Oxygen Reduction Reaction

Journal Article · 25 October 2023 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.3c03998 · OSTI ID:2281115

Peles-Strahl, Leigh ^[1]; Honig, Hilah C. ^[2]; Persky, Yeela ^[2];

^[3]; Dahan, Adi ^[4];

^[2]

Bar-Ilan Univ., Ramat Gan (Israel); Israel Atomic Energy Commission (IAEC), Yavne (Israel). Soreq Nuclear Research Centre (Soreq NRC)
Bar-Ilan Univ., Ramat Gan (Israel)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Israel Atomic Energy Commission (IAEC), Yavne (Israel). Soreq Nuclear Research Centre (Soreq NRC)

Aerogels have a large surface area and a porous structure, which make them an attractive catalyst support materials for fuel cells. Modifying the aerogels’ building blocks and introducing catalytic sites into their backbones allow them to function as both catalysts and supports, thereby increasing the density and distribution of catalyst active sites. In this work, we studied conjugated aerogels containing iron–bipyridine catalytic sites for the oxygen reduction reaction. To demonstrate the variation in physical and electrochemical properties of these aerogels, a series of aerogels were synthesized by a Glaser coupling reaction. Iron salt was added to the three-dimensional gel to produce iron–bipyridine complexes and obtain atomically dispersed catalytic sites. The electrocatalytic activity and electrical conductivity of the aerogels were increased after their heat treatment to yield Fe-doped carbon aerogels. The control of metal loadings was accomplished by changing the bipyridine content during the aerogel synthesis, resulting in 0.9–4.1 wt % Fe. In conclusion, the results show a correlation between Fe loading, aerogel structure, and catalytic activity, achieving high performance for the oxygen reduction reaction in both acidic and alkaline media.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2281115

Journal Information:: ACS Catalysis, Vol. 13, Issue 21; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (49)

Molecular metal nanoclusters for ORR, HER and OER: Achievements, opportunities and challenges Qin, Dong-Dong; Tang, Yun; Ma, Guanyu International Journal of Hydrogen Energy, Vol. 46, Issue 51 https://doi.org/10.1016/j.ijhydene.2021.05.096	journal	July 2021
Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects Matanovic, Ivana; Artyushkova, Kateryna; Strand, Matthew B. The Journal of Physical Chemistry C, Vol. 120, Issue 51 https://doi.org/10.1021/acs.jpcc.6b09778	journal	December 2016
In situ electrochemical quantification of active sites in Fe–N/C non-precious metal catalysts Malko, Daniel; Kucernak, Anthony; Lopes, Thiago Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13285	journal	October 2016
Quantifying the electrochemical active site density of precious metal-free catalysts in situ in fuel cells Snitkoff-Sol, Rifael Z.; Friedman, Ariel; Honig, Hilah C. Nature Catalysis, Vol. 5, Issue 2 https://doi.org/10.1038/s41929-022-00748-9	journal	February 2022
The Analysis of Copper-Iron Metallic Mixture by Means of XRD and XRF Omar, Halo Dalshad International Letters of Chemistry, Physics and Astronomy, Vol. 64 https://doi.org/10.56431/p-tj32k9	journal	February 2016
Renewable energy communities under the 2019 European Clean Energy Package – Governance model for the energy clusters of the future? Lowitzsch, J.; Hoicka, C. E.; van Tulder, F. J. Renewable and Sustainable Energy Reviews, Vol. 122 https://doi.org/10.1016/j.rser.2019.109489	journal	April 2020
A class of non-precious metal composite catalysts for fuel cells Bashyam, Rajesh; Zelenay, Piotr Nature, Vol. 443, Issue 7107 https://doi.org/10.1038/nature05118	journal	September 2006
Platinum group metal-free catalysts boost cost competitiveness of fuel cell vehicles Thompson, Simon T.; Papageorgopoulos, Dimitrios Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0291-x	journal	July 2019
Methods for assessment and measurement of the active site density in platinum group metal–free oxygen reduction reaction catalysts Kozhushner, Alisa; Zion, Noam; Elbaz, Lior Current Opinion in Electrochemistry, Vol. 25 https://doi.org/10.1016/j.coelec.2020.08.002	journal	February 2021
Designing the next generation of proton-exchange membrane fuel cells Jiao, Kui; Xuan, Jin; Du, Qing Nature, Vol. 595, Issue 7867 https://doi.org/10.1038/s41586-021-03482-7	journal	July 2021
Gasoline automobile catalysis and its historical journey to cleaner air Farrauto, Robert J.; Deeba, Michel; Alerasool, Saeed Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0312-9	journal	July 2019
Toward Platinum Group Metal-Free Catalysts for Hydrogen/Air Proton-Exchange Membrane Fuel Cells Jaouen, Frédéric; Jones, Deborah; Coutard, Nathan Johnson Matthey Technology Review, Vol. 62, Issue 2 https://doi.org/10.1595/205651318X696828	journal	April 2018
Synthesis–structure–performance correlation for polyaniline–Me–C non-precious metal cathode catalysts for oxygen reduction in fuel cells Wu, Gang; Johnston, Christina M.; Mack, Nathan H. Journal of Materials Chemistry, Vol. 21, Issue 30 https://doi.org/10.1039/c0jm03613g	journal	January 2011
Bipyridine Modified Conjugated Carbon Aerogels as a Platform for the Electrocatalysis of Oxygen Reduction Reaction Peles‐Strahl, Leigh; Zion, Noam; Lori, Oran Advanced Functional Materials, Vol. 31, Issue 26 https://doi.org/10.1002/adfm.202100163	journal	April 2021
An ultralight, supercompressible, superhydrophobic and multifunctional carbon aerogel with a specially designed structure Long, Sishi; Feng, Yunchao; He, Faliang Carbon, Vol. 158 https://doi.org/10.1016/j.carbon.2019.11.065	journal	March 2020
Application of Molecular Catalysts for the Oxygen Reduction Reaction in Alkaline Fuel Cells Friedman, Ariel; Mizrahi, Michal; Levy, Naomi ACS Applied Materials & Interfaces, Vol. 13, Issue 49 https://doi.org/10.1021/acsami.1c16311	journal	December 2021
Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction Cai, Bin; Hübner, René; Sasaki, Kotaro Angewandte Chemie International Edition, Vol. 57, Issue 11 https://doi.org/10.1002/anie.201710997	journal	February 2018
Accurate Evaluation of Active-Site Density (SD) and Turnover Frequency (TOF) of PGM-Free Metal–Nitrogen-Doped Carbon (MNC) Electrocatalysts using CO Cryo Adsorption Luo, Fang; Choi, Chang Hyuck; Primbs, Mathias J. M. ACS Catalysis, Vol. 9, Issue 6 https://doi.org/10.1021/acscatal.9b00588	journal	April 2019
Homogenous Electrocatalytic Oxygen Reduction Rates Correlate with Reaction Overpotential in Acidic Organic Solutions Pegis, Michael L.; McKeown, Bradley A.; Kumar, Neeraj ACS Central Science, Vol. 2, Issue 11 https://doi.org/10.1021/acscentsci.6b00261	journal	October 2016
Chemical and Electrochemical O₂ Reduction on Earth-Abundant M-N-C Catalysts and Implications for Mediated Electrolysis Bates, Jason S.; Biswas, Sourav; Suh, Sung-Eun Journal of the American Chemical Society, Vol. 144, Issue 2 https://doi.org/10.1021/jacs.1c11126	journal	January 2022
Bioinspired Electrocatalysis of Oxygen Reduction Reaction in Fuel Cells Using Molecular Catalysts Zion, Noam; Friedman, Ariel; Levy, Naomi Advanced Materials, Vol. 30, Issue 41 https://doi.org/10.1002/adma.201800406	journal	April 2018
Recent Advances on Electrocatalysis Using Pristinely Conductive Metal‐Organic Frameworks and Covalent Organic Frameworks Guan, Yiran; Lai, Jianping; Xu, Guobao ChemElectroChem, Vol. 8, Issue 15 https://doi.org/10.1002/celc.202100492	journal	June 2021
Metallocorroles as Non-Precious Metal Electrocatalysts for Highly Efficient Oxygen Reduction in Alkaline Media Levy, Naomi; Mahammed, Atif; Friedman, Ariel ChemCatChem, Vol. 8, Issue 17 https://doi.org/10.1002/cctc.201600556	journal	August 2016
Microstructure and strengthening mechanisms in Cu/Fe multilayers Chen, Y.; Liu, Y.; Sun, C. Acta Materialia, Vol. 60, Issue 18 https://doi.org/10.1016/j.actamat.2012.08.005	journal	October 2012
PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises He, Yanghua; Wu, Gang Accounts of Materials Research, Vol. 3, Issue 2 https://doi.org/10.1021/accountsmr.1c00226	journal	January 2022
Electrocatalysis of Oxygen Reduction Reaction in a Polymer Electrolyte Fuel Cell with a Covalent Framework of Iron Phthalocyanine Aerogel Zion, Noam; Peles-Strahl, Leigh; Friedman, Ariel ACS Applied Energy Materials, Vol. 5, Issue 7 https://doi.org/10.1021/acsaem.2c00375	journal	July 2022
Porphyrin Aerogel Catalysts for Oxygen Reduction Reaction in Anion‐Exchange Membrane Fuel Cells Zion, Noam; Douglin, John C.; Cullen, David A. Advanced Functional Materials, Vol. 31, Issue 24 https://doi.org/10.1002/adfm.202100963	journal	April 2021
A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts Marshall-Roth, Travis; Libretto, Nicole J.; Wrobel, Alexandra T. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-18969-6	journal	October 2020
Design of advanced aerogel structures for oxygen reduction reaction electrocatalysis Peles‐Strahl, Leigh; Persky, Yeela; Elbaz, Lior SusMat, Vol. 3, Issue 1 https://doi.org/10.1002/sus2.104	journal	January 2023
Mapping transition metal–nitrogen–carbon catalyst performance on the critical descriptor diagram Specchia, Stefania; Atanassov, Plamen; Zagal, José H. Current Opinion in Electrochemistry, Vol. 27 https://doi.org/10.1016/j.coelec.2021.100687	journal	June 2021
In Situ Mechanistic Investigation of O ₂ Reduction by Iron Porphyrin Electrocatalysts Using Surface-Enhanced Resonance Raman Spectroscopy Coupled to Rotating Disk Electrode (SERRS-RDE) Setup Sengupta, Kushal; Chatterjee, Sudipta; Dey, Abhishek ACS Catalysis, Vol. 6, Issue 10 https://doi.org/10.1021/acscatal.6b01122	journal	September 2016
Hydrogen in energy transition: A review Kovač, Ankica; Paranos, Matej; Marciuš, Doria International Journal of Hydrogen Energy, Vol. 46, Issue 16 https://doi.org/10.1016/j.ijhydene.2020.11.256	journal	March 2021
Promoting Electrocatalysis upon Aerogels Cai, Bin; Eychmüller, Alexander Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201804881	journal	December 2018
Heat‐Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction Zion, Noam; Cullen, David A.; Zelenay, Piotr Angewandte Chemie International Edition, Vol. 59, Issue 6 https://doi.org/10.1002/anie.201913521	journal	February 2020
Optimizing the Pd Sites in Pure Metallic Aerogels for Efficient Electrocatalytic H₂O₂ Production Zhang, Xin; Wang, Cui; Chen, Kai Advanced Materials, Vol. 35, Issue 14 https://doi.org/10.1002/adma.202211512	journal	March 2023
Assessing and measuring the active site density of PGM-free ORR catalysts Snitkoff-Sol, Rifael Z.; Elbaz, Lior Journal of Solid State Electrochemistry, Vol. 26, Issue 9 https://doi.org/10.1007/s10008-022-05236-5	journal	July 2022
Simplified FTacV model to quantify the electrochemically active site density in PGM-free ORR catalysts Friedman, Ariel; Snitkoff-Sol, Rifael Z.; Honig, Hilah C. Electrochimica Acta, Vol. 463 https://doi.org/10.1016/j.electacta.2023.142865	journal	September 2023
Recent advances in high‐loading catalysts for low‐temperature fuel cells: From nanoparticle to single atom Shen, Lixiao; Ma, Miao; Tu, Fengdi SusMat, Vol. 1, Issue 4 https://doi.org/10.1002/sus2.38	journal	December 2021
Progress in the Development of Fe‐Based PGM‐Free Electrocatalysts for the Oxygen Reduction Reaction Martinez, Ulises; Komini Babu, Siddharth; Holby, Edward F. Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201806545	journal	December 2018
Misconceptions in interpretation of nitrogen chemistry from x-ray photoelectron spectra Artyushkova, Kateryna Journal of Vacuum Science & Technology A, Vol. 38, Issue 3 https://doi.org/10.1116/1.5135923	journal	May 2020
Metallocorroles as Nonprecious-Metal Catalysts for Oxygen Reduction Levy, Naomi; Mahammed, Atif; Kosa, Monica Angewandte Chemie International Edition, Vol. 54, Issue 47 https://doi.org/10.1002/anie.201505236	journal	October 2015
Molecular Design of Single‐Atom Catalysts for Oxygen Reduction Reaction Wan, Chengzhang; Duan, Xiangfeng; Huang, Yu Advanced Energy Materials, Vol. 10, Issue 14 https://doi.org/10.1002/aenm.201903815	journal	February 2020
Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction in PEM Fuel Cells: Self-Template Synthesis Approach to Enhancing Catalytic Activity and Stability He, Yanghua; Tan, Qiang; Lu, Leilei Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00031-9	journal	March 2019
Selective Hydroxylation of Benzene to Phenol over Fe Nanoparticles Encapsulated within N-Doped Carbon Shells Lu, Erjun; Wu, Jiancong; Yang, Baoying ACS Applied Nano Materials, Vol. 3, Issue 9 https://doi.org/10.1021/acsanm.0c01824	journal	August 2020
Just a Dream—or Future Reality? Gasteiger, Hubert A.; Marković, Nenad M Science, Vol. 324, Issue 5923, p. 48-49 https://doi.org/10.1126/science.1172083	journal	April 2009
A review of heat-treatment effects on activity and stability of PEM fuel cell catalysts for oxygen reduction reaction Bezerra, Cicero W. B.; Zhang, Lei; Liu, Hansan Journal of Power Sources, Vol. 173, Issue 2 https://doi.org/10.1016/j.jpowsour.2007.08.028	journal	November 2007
State-of-the-art and developmental trends in platinum group metal-free cathode catalyst for anion exchange membrane fuel cell (AEMFC) Hossen, Md. Mosaddek; Hasan, Md. Shamim; Sardar, Md. Riajul Islam Applied Catalysis B: Environmental, Vol. 325 https://doi.org/10.1016/j.apcatb.2022.121733	journal	May 2023
A hydrogen economy: opportunities and challenges Tseng, Phillip; Lee, John; Friley, Paul Energy, Vol. 30, Issue 14 https://doi.org/10.1016/j.energy.2004.07.015	journal	November 2005
Review on hydrogen storage materials and methods from an electrochemical viewpoint Kaur, Manmeet; Pal, Kaushik Journal of Energy Storage, Vol. 23 https://doi.org/10.1016/j.est.2019.03.020	journal	June 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
aerogels
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electrocatalysis
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Title: Modular Iron–Bipyridine-Based Conjugated Aerogels as Catalysts for Oxygen Reduction Reaction

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References (49)

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