O‐, N‐Atoms‐Coordinated Mn Cofactors within a Graphene Framework as Bioinspired Oxygen Reduction Reaction Electrocatalysts

Yang, Yang; Mao, Kaitian; Gao, Shiqi; Huang, Hao; Xia, Guoliang; Lin, Zhiyu; Jiang, Peng; Wang, Changlai; Wang, Hui; Chen, Qianwang

doi:10.1002/adma.201801732

Cited by 268 publications

(233 citation statements)

References 51 publications

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“…As shown by the HAADF‐STEM images and EDX mapping results, the Co, Ni, and Mn single atoms with high concentration were uniformly distributed on the HCF (Figure 4b–d,g–i,l–n). The binding energies of Co, Ni, and Mn in XPS spectra were similar with those of the previously reported Co‐N‐C, Ni‐N‐C, and Mn‐N‐C single atoms (Figure 4e,j,o), respectively . Determined by the XPS results, the mass percentage of Co, Ni, and Mn single atoms were calculated to be 3.7%, 4.2%, and 2.6%, respectively (Figure S16 and Table S4, Supporting Information).…”

Section: Resultssupporting

confidence: 85%

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Lei

Liu

Yin

et al. 2020

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Increasing the mass loading of transition metal single atoms coordinated with nitrogen in carbon‐based materials (M‐N‐C) is still challenging. Herein, inspired by the bioconcentration effect in the living body, a biochemistry strategy for the synthesis of Fe‐N‐C single atoms is demonstrated. Through introducing ferrous glycinate into the growth of fungus, the Fe atoms are bioconcentrated in hyphae. The highly dispersed Fe‐N‐C single atoms in hyphae‐derived carbon fibers (labeled as Fe‐N‐C SA/HCF) are prepared by the pyrolysis of Fe‐riched hyphae. In the bioconcentration process, the uptake of Fe ions by hyphae promotes the secretion of glutathione and ferritin, which provides additional coordination sites for Fe ions. Accordingly, the mass content of Fe in bioconcentrated Fe‐N‐C SA/HCF reaches 4.8%, which is 5.3 times larger than that of the sample prepared by the conventional pyrolysis process. The present bioconcentration strategy is further extended to the preparation of Co, Ni, and Mn single atoms. Owing to the high content of Fe‐N‐C single atoms, Fe‐N‐C SA/HCF shows the onset potential (Eonset) of 0.931 V versus reversible hydrogen electrode (RHE) and half‐wave potential (E1/2) of 0.802 V versus RHE in oxygen reduction reaction measurements, which is comparable to the commercial Pt/C catalysts.

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Section: Resultssupporting

confidence: 85%

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Lei

Liu

Yin

et al. 2020

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“…Similar to N‐coordination, the coordinated O atoms also play a significant role in tuning the catalytic activity of the metal center. The N‐, O‐coordinated Mn SACs have been synthesized and exhibit encouraging ORR performance in alkaline condition . DFT calculations reveal that the improvement in activity of Mn atoms should be ascribed to the tuning of the local density of states (DOS) of the Mn d‐orbitals via the change in the nearby electronic environment.…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

281

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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“…Various sites of the catalysts have been verified active in the reaction of the ORR process, including metal–sulfur bonding, metal–oxygen bonding, oxygen vacancy, and so on 60,137…”

Section: Orr Performance and Active Site Researchmentioning

confidence: 99%

Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species

Huang

Shen

Zhang

et al. 2019

Advanced Energy Materials

188

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Developing substitutes of noble metal catalysts toward oxygen reduction reaction (ORR) at the cathode is of vital importance for promoting low‐temperature polymer electrolyte membrane fuel cells. Transition metal species have been one of the hot areas of interest due to their low cost, high activity, and long‐term stability. The design of porous carbon nanostructures decorated with transition metal species plays a vital role in enhancing ORR catalytic performance. Here, the recent breakthroughs in porous carbon nanostructures decorated with transition metal species (including nanoparticles and atomically dispersed supported metal) are discussed. The porous nanostructures can provide large surface area as well as abundant pore channels, leading to sufficient exposure of active sites and efficient mass transfer. These nanostructures can be synthesized by several approaches, including the templated method, the self‐templated method, the impregnation process, and so on. Furthermore, the ORR performance and the exploration of active sites are also discussed for further enhancement of the ORR catalysts. Finally, the challenges and prospects are discussed, which would push forward the development of ORR catalysts in the near future.

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O‐, N‐Atoms‐Coordinated Mn Cofactors within a Graphene Framework as Bioinspired Oxygen Reduction Reaction Electrocatalysts

Cited by 268 publications

References 51 publications

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species

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