A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts

Zhu, Youqi; Sun, Wenming; Luo, Jun; Chen, Wenxing; Cao, Tai; Zheng, Lirong; Dong, Juncai; Zhang, Jian; Zhang, Maolin; Han, Yunhu; Chen, Chen; Peng, Qing; Wang, Dingsheng; Li, Yadong

doi:10.1038/s41467-018-06296-w

Cited by 232 publications

(169 citation statements)

References 80 publications

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“…In addition, Li and co‐workers reported a new strategy using cocoon silk chemistry to synthetize single metal catalysts anchored on N‐doped carbon nanosheets with porous structure and high defects. They proposed that Co‐N 4 sites were the greatest possible coordination structures for Co atoms and served as the main active sites in Co‐ISA/CNS catalyst …”

Section: Defects‐based Single Atomic Electrocatalystmentioning

confidence: 99%

Defect‐Based Single‐Atom Electrocatalysts

et al. 2018

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Single‐atom catalysts (SACs) have attracted great attention owing to their maximum atomic utilization and high catalytic performance in electrochemical reactions. But the synthesis of SACs is not easy due to large surface energies of single atomic metal sites which often lead to their aggregation. The defects on supports can serve as anchor sites to stabilize single metal atoms and prevent them from aggregation, which has become an effective method to fabricate SACs. This review summarizes the meaningful findings about the defects on supports stabilizing single metal atoms, and their applications in electrocatalytic reaction. Various defects, including the intrinsic defects or heteroatom doping of carbon‐based materials, cation or anion vacancies of metal compound supports, and other defects (step edges, lattice defects, and caves), are comprehensively summarized, and the effects of defects on designing SACs are discussed. Although there are still many challenges to fully explore the SACs, it is believed that the newly established defect sites stabilized single atoms mechanism will be helpful for designing and fabricating highly powerful single atomic electrocatalysts for practical applications.

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Section: Defects‐based Single Atomic Electrocatalystmentioning

confidence: 99%

Defect‐Based Single‐Atom Electrocatalysts

et al. 2018

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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: Resultsmentioning

confidence: 99%

“…Through the conformational change, the protein is able to bind isolated metal ion, which prevents the aggregation of single atoms . For example, a cocoon silk chemistry strategy has recently been developed for the preparation of metal single atoms . In living body, the uptake of metal ions promotes the formation of proteins, which allows additional coordinated metal ions located in living body (denoted as bioconcentration phenomenon).…”

Section: Introductionmentioning

confidence: 99%

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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“…In addition, X‐ray absorption fine structure (XANFS) is known for accurately reflecting the oscillatory structure of the samples according to the X‐ray absorption coefficient . It generally includes X‐ray absorption near edge structure (XANES) and extended X‐ray absorption fine structure (EXAFS).…”

Section: Fabrication Strategies and Characteristic Methods Of Sagmentioning

confidence: 99%

Single Atoms on Graphene for Energy Storage and Conversion

et al. 2019

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Single atoms are attracting much attention in the field of energy conversion and storage due to their maximal atomic utilization, high efficiency, and good selectivity. Moreover, their unique electronic structure could improve the intrinsic activity of the active sites. However, the high surface free energy of single atoms inevitably results in their serious aggregation, leading to degraded catalytic activity and poor cycling life. To solve these issues, supports with high surface areas have to be developed to reduce loading density of single atoms and further decrease the surface free energy. Furthermore, engineering the active sites of these substrates can also regulate chemical coordination of single atoms, enhancing their catalytic performance. Owing to high surface area, excellent conductivity and adjustable surface properties, graphene is widely utilized to load atomic metal catalysts. In this review, the fabrication strategies and characterization methods of single atoms on graphene (SAG) are summarized first. Subsequently, the electrochemical applications of SAG on the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction, and methane oxidation are discussed in detail. Finally, the future developments and prospects in fabrication and application of SAG are also discussed.

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A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts

Cited by 232 publications

References 80 publications

Defect‐Based Single‐Atom Electrocatalysts

Defect‐Based Single‐Atom Electrocatalysts

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Single Atoms on Graphene for Energy Storage and Conversion

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