A CeO2 modified phenylenediamine-based Fe/N/C with enhanced durability/stability as non-precious metal catalyst for oxygen reduction reaction

Wei, Houwei; Su, Xiaogang; Liu, Jianguo; Tian, Juan; Wang, Zhongwei; Sun, Kui; Zhang, Rui; Yang, Weiwei; Zou, Zhigang

doi:10.1016/j.elecom.2018.01.011

Cited by 47 publications

(19 citation statements)

References 25 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In view of the electronic interaction effect, modification of transition metal‐based catalysts with foreign promoters should be a reliable strategy to regulate their electrocatalytic performance 33–37. Recently, rare earth oxides (REO) have attracted special interest as the foreign promoters to modulate the electrocatalytic properties of various transition metals33,38–42 owing to their unique electronic and chemical properties of 4f subshell electrons 43,44. As demonstrated by Shao and co‐workers,39 the ORR activity of Co 3 O 4 /ketjenblack could be significantly improved by doping with CeO 2 REO.…”

Section: Introductionmentioning

confidence: 99%

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Wang

Yang

et al. 2020

Advanced Energy Materials

135

View full text Add to dashboard Cite

Rare earth doped materials with unique electronic ground state configurations are considered emerging alternatives to conventional Pt/C for the oxygen reduction reaction (ORR). Herein, gadolinium (Gd)‐induced valence structure engineering is, for the first, time investigated for enhanced oxygen electrocatalysis. The Gd2O3–Co heterostructure loaded on N‐doped graphene (Gd2O3–Co/NG) is constructed as the target catalyst via a facile sol–gel assisted strategy. This synthetic strategy allows Gd2O3–Co nanoparticles to distribute uniformly on an N‐graphene surface and form intimate Gd2O3/Co interface sites. Upon the introduction of Gd2O3, the ORR activity of Gd2O3–Co/NG is significantly increased compared with Co/NG, where the half‐wave potential (E1/2) of Gd2O3–Co/NG is 100 mV more positive than that of Co/NG and even close to commercial Pt/C. The density functional theory calculation and spectroscopic analysis demonstrate that, owing to intrinsic charge redistribution at the engineered interface of Gd2O3/Co, the coupled Gd2O3–Co can break the OOH*–OH* scaling relation and result in a good balance of OOH* and OH* binding on Gd2O3–Co surface. For practical application, a rechargeable Zn–air battery employing Gd2O3–Co/NG as an air–cathode achieves a large power density and excellent charge–discharge cycle stability.

show abstract

Section: Introductionmentioning

confidence: 99%

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Wang

Yang

et al. 2020

Advanced Energy Materials

135

View full text Add to dashboard Cite

show abstract

“…These results indicate that due to the lack of inducing effect of CeO 2 during the synthesis of FeÀ N/C sample, the ORR activities of the FeÀ N/C catalyst can only be improved finitely through adding CeO 2 after FeÀ N/C synthesis. Besides, the proper adding amount of CeO 2 can also eliminate the production of intermediates such as H 2 O 2 during the catalytic reaction, [47] and increase the retention rate of catalytically active sites, thereby improving the stability of FeÀ N/CÀ CeO 2 catalyst.…”

Section: Resultsmentioning

confidence: 99%

“…[45] Furthermore, it is worth mentioning that there also exists an electronic interaction between CeO 2 and metal in the co-synthesized catalyst, which may enhance the oxygen absorption on the catalyst for improved ORR activity. [46] Besides, CeO 2 can effectively catalyze the decomposition of H 2 O 2 , which is very favorable for the retention of active sites in ORR catalysts, [47] thereby improving the long-term stability. [48,49] Considering all the benefits, CeO 2 can be combined with other materials to design novel ORR catalysts.…”

Section: Introductionmentioning

confidence: 99%

“…[50][51][52][53] However, in spite of the fact that the CeO 2 loading is a feasible strategy for designing ORR electrocatalysts, the relative content of CeO 2 as a co-catalyst is a pivotal factor for the enhanced catalytic activities. [47,[54][55][56] For example, excessive loading amount may lead to the aggregation of CeO 2 nanoparticles and hinder the exposure of the active site as well, which results in a decrease of the electrocatalytic performance on the contrary.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Fabricating Nitrogen‐Rich Fe−N/C Electrocatalysts through CeO₂‐Assisted Pyrolysis for Enhanced Oxygen Reduction Reaction

et al. 2019

View full text Add to dashboard Cite

The electrochemical oxygen reduction reaction (ORR) is a central process of various energy conversion systems. Yet, searching non‐noble‐metal electrocatalysts with superior ORR performance is still a great challenge. Herein, CeO2‐loaded Fe−N/C catalysts (Fe−N/C−CeO2) were prepared through a facile hydrothermal and pyrolysis method for enhanced ORR properties. The proper amount of CeO2 can induce the anchoring of N species during the pyrolysis process, and increase the N‐containing active sites such as Fe−Nx. Moreover, CeO2 nanoparticles are capable of rapidly reducing the H2O2 intermediate in ORR, further boosting the durability of the catalyst. Consequently, the Fe−N/C−CeO2 (1 %) catalyst delivers prominent ORR performance with a half‐wave potential of 0.862 V and a diffusion limiting current density of 5.51 mA cm−2 in 0.1 M KOH, which is superior than that of the Fe−N/C catalyst, and even comparable to that of commercial Pt/C catalyst. Furthermore, the long‐term stability test of Fe−N/C−CeO2 (1 %) shows a negative shift of just 18 mV of the half‐wave potential after 10000 cycles, which is much smaller than that of the Fe−N/C sample.

show abstract

“…Selecting additives for PGM-free catalysts such as CeO2 to consume hydrogen peroxide is another alternative way to enhance stability performance. Zou's group 105 incorporated CeO2 in the catalyst to significantly reduce the production of H2O2, saving a 50% loss of E1/2 in the stability test. The mechanism was illustrated by the following reactions:…”

Section: The Corrosion Of the Carbon Supportmentioning

confidence: 99%

Recent Progress in Proton-Exchange Membrane Fuel Cells Based on Metal-Nitrogen-Carbon Catalysts

丁亮¹,

Tang²,

胡劲松³

2020

Acta Physico Chimica Sinica

View full text Add to dashboard Cite

Proton-exchange membrane fuel cells (PEMFCs) directly transform chemical energy into electrical energy with high energy density and zero carbon emissions, thereby offering a clean energy alternative for fossil fuels and vehicle electrification. However, the existing PEMFCs rely on Pt-based catalysts, especially at the cathode side wherein the sluggish oxygen reduction reaction (ORR) takes place, resulting in high cost and limiting their commercial applications. Therefore, there is a strong interest in developing platinum group metal-free (PGM-free) PEMFCs. Although impressive advancements have been made since metalnitrogen-carbon (M-N-C) catalysts have been developed as promising candidates for low-cost cathode catalysts, PGM-free PEMFCs still suffer from insufficient activity and durability. Owing to the intricate structure of the tri-phase interface and mass transport limitation, the M-N-C catalysts with high ORR activity in rotating disk electrode (RDE) tests still suffer from unexpected problems such as showing low activity and undesired rapid degradation process in real fuel cell conditions. Therefore, a comprehensive understanding of the active sites and influences of the M-N-C catalyst structure and cathode structure on the PEMFC performance will promote the development of PGM-free PEMFCs. Herein, with an aim to increase the activity and durability of PEMFCs based on M-N-C catalysts, we summarize the recent progress in understanding the active sites of M-N-C catalysts and the relationships between the structures of catalysts/catalyst layers and device performances. At the catalyst level, multiple delicately designed synthetic strategies suggest that attractive device performances can be obtained by tailoring the intrinsic activity and density of the catalyst active sites while engineering the porosity of catalysts to improve the utilization of active sites. Additionally, integrating the catalyst ink into the cathode catalyst layers in PGM-free PEMFC is pivotal for transforming the impressive ORR performance of catalysts in the RDE test to fuel cell performance. Accordingly, the recent advances in the enhancement of mass transfer and charge transport to achieve remarkable fuel cell performance were also included by rationally designing ionomer contents, catalyst morphology, and fabrication process of cathodic catalyst layers. Moreover, durability is the Achilles heel of PEMFCs with M-N-C catalysts, which is currently far behind the commercial requirements. The possible degradation mechanisms and the recent progress in seeking the corresponding solutions are also discussed in this review, including the decomposition of metal species, protonation of nitrogen sites, corrosion of carbon support, and micropore flooding. Based on these insights, the perspective is proposed by articulating open challenges and opportunities in materials innovations and device engineering with an aim to achieve practical M-N-C based PEMFCs.

show abstract

A CeO2 modified phenylenediamine-based Fe/N/C with enhanced durability/stability as non-precious metal catalyst for oxygen reduction reaction

Cited by 47 publications

References 25 publications

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Fabricating Nitrogen‐Rich Fe−N/C Electrocatalysts through CeO₂‐Assisted Pyrolysis for Enhanced Oxygen Reduction Reaction

Recent Progress in Proton-Exchange Membrane Fuel Cells Based on Metal-Nitrogen-Carbon Catalysts

Contact Info

Product

Resources

About

A CeO2 modified phenylenediamine-based Fe/N/C with enhanced durability/stability as non-precious metal catalyst for oxygen reduction reaction

Cited by 47 publications

References 25 publications

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis

Fabricating Nitrogen‐Rich Fe−N/C Electrocatalysts through CeO2‐Assisted Pyrolysis for Enhanced Oxygen Reduction Reaction

Recent Progress in Proton-Exchange Membrane Fuel Cells Based on Metal-Nitrogen-Carbon Catalysts

Contact Info

Product

Resources

About

Fabricating Nitrogen‐Rich Fe−N/C Electrocatalysts through CeO₂‐Assisted Pyrolysis for Enhanced Oxygen Reduction Reaction