High-Density Planar-like Fe2N6 Structure Catalyzes Efficient Oxygen Reduction

Zhang, Nan; Zhou, Tianshou; Ge, Jiankai; Lin, Yue; Du, Zhiyi; Zhong, Cheng’an; Wang, Wenjie; Jiao, Qiyang; Yuan, Ruilin; Tian, Yangchao; Chu, Wangsheng; Wu, Changzheng; Xie, Yi

doi:10.1016/j.matt.2020.06.026

Cited by 207 publications

(173 citation statements)

References 41 publications

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“…Meanwhile, the higher white line intensity of FeNi SAs/NCs also confirms that Fe is more positively charged and indicates a strong interaction between the heteronuclear Fe‐Ni atoms and the defective nitrogen‐doped carbon matrix. [ 32,41 ] Moreover, the variation trend of the white line intensity is consistent with that of the M‐N/O coordination number, and the enhanced white line intensity can be attributed to the increased percentage of single atomic and proposed single atomic structures, further demonstrating that atomic‐level metal structures can effectively adjust the properties of electrons. In the k 3 ‐weighted Fourier transform (FT)‐EXAFS spectra in the R‐space (Figure 2d), as expected, FeNi SAs/NC exhibits two strong peaks at 1.50 and 2.27 Å, corresponding to Fe‐N and metal–metal bonds, respectively.…”

Section: Resultssupporting

confidence: 52%

Dual‐Sites Coordination Engineering of Single Atom Catalysts for Flexible Metal–Air Batteries

Yun

et al. 2021

Advanced Energy Materials

307

174

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Dual‐sites single atom catalysts hold promise for efficiently regulating multiple reaction processes and explicitly explaining the underlying mechanisms. However, delicate atomic engineering for dual‐site single atom catalysts remains a huge challenge. Herein, atomically dispersed Fe‐Ni single atoms embedded in a nitrogen‐doped carbon matrix (FeNi SAs/NC) are successfully developed with extraordinary activity for electrocatalytic oxygen reduction and evolution reactions (ORR/OER). The atomic FeNi SAs/NC catalyst displays high onset potential (0.98 V) and half‐wave potential (0.84 V) for the ORR, as well as, low overpotential of (270 mV) at 10 mA cm−2 for the OER. The density functional theory calculations indicate that the Fe site as the active center can facilitate the four‐electron reaction process, while Ni sites regulate the electronic structure of Fe sites and further reduce the energy barrier of the rate‐determining step. In addition, the nitrogen‐doped carbon matrix prevents the metal atoms from aggregation and corrosion, leading to the improvement of catalyst durability. As a proof of concept, flexible quasi‐solid‐state zinc– and aluminum–air batteries assembled with the FeNi SAs/NC catalyst exhibit superior peak power densities and discharging specific capacities outperforming the commercial Pt/C. This work provides rational guidance for the synthesis of bifunctional electrocatalysts in next‐generation energy devices for flexible consumer electronics.

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Section: Resultssupporting

confidence: 52%

Dual‐Sites Coordination Engineering of Single Atom Catalysts for Flexible Metal–Air Batteries

Yun

et al. 2021

Advanced Energy Materials

307

174

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“…Zhang et al also reported that Fe 2 N 6 was more active than FeN 4 in catalyzing ORR. [142] Table 1 summarizes the activity of various SACs for 2e − and 4e − ORR.…”

Section: Dual Metal Active Centermentioning

confidence: 99%

Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Zhang

Yang

Liu

2020

Advanced Energy Materials

268

185

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Future renewable energy supplies and a sustainable environment rely on many important catalytic processes. Single‐atom catalysts (SACs) are attractive because of their maximum atom utilization efficiency, tunable electronic structures, and outstanding catalytic performance. Of particular note, transition‐metal SACs exhibit excellent catalytic activity and selectivity for the oxygen reduction reaction (ORR)—an important half reaction in fuel cells and metal–air batteries as well as for portable hydrogen peroxide (H2O2) production. Although considerable efforts have been made on the synthesis of SACs for ORR, the regulation of the coordination environments of SACs and thus the electronic structures still pose a big challenge. In this review, strategies for manipulating the coordination environments of SACs are classified into three categories, including regulation of the center metal atoms, manipulation of the surrounding environment connecting to the center metal atom, and modification of the geometric configuration of the support. Finally, some issues regarding the future development of SACs for ORR are raised and possible solutions are proposed.

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“…The oxygen reduction reaction (ORR), represents the cornerstone for regenerative energy conversion devices involving polymer electrolyte membrane fuel cell (PEMFC) and metal–air batteries 1 – 7 . Hitherto, the generally recognized state-of-the-art platinum (Pt)-based catalysts possess the highest kinetic activity in catalyzing ORR under acid and alkaline media, however, the scarcity, price, and low methanol crossover tolerance of Pt alloys have motivated the search for cost-effective non-noble-metal electrocatalysts 8 – 13 .…”

Section: Introductionmentioning

confidence: 99%

Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity

et al. 2021

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As low-cost electrocatalysts for oxygen reduction reaction applied to fuel cells and metal-air batteries, atomic-dispersed transition metal-nitrogen-carbon materials are emerging, but the genuine mechanism thereof is still arguable. Herein, by rational design and synthesis of dual-metal atomically dispersed Fe,Mn/N-C catalyst as model object, we unravel that the O2 reduction preferentially takes place on FeIII in the FeN4 /C system with intermediate spin state which possesses one eg electron (t2g4eg1) readily penetrating the antibonding π-orbital of oxygen. Both magnetic measurements and theoretical calculation reveal that the adjacent atomically dispersed Mn-N moieties can effectively activate the FeIII sites by both spin-state transition and electronic modulation, rendering the excellent ORR performances of Fe,Mn/N-C in both alkaline and acidic media (halfwave positionals are 0.928 V in 0.1 M KOH, and 0.804 V in 0.1 M HClO4), and good durability, which outperforms and has almost the same activity of commercial Pt/C, respectively. In addition, it presents a superior power density of 160.8 mW cm−2 and long-term durability in reversible zinc–air batteries. The work brings new insight into the oxygen reduction reaction process on the metal-nitrogen-carbon active sites, undoubtedly leading the exploration towards high effective low-cost non-precious catalysts.

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High-Density Planar-like Fe2N6 Structure Catalyzes Efficient Oxygen Reduction

Cited by 207 publications

References 41 publications

Dual‐Sites Coordination Engineering of Single Atom Catalysts for Flexible Metal–Air Batteries

Dual‐Sites Coordination Engineering of Single Atom Catalysts for Flexible Metal–Air Batteries

Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity

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