Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

Guo, J.; Huo, Juanjuan; Liu, Yan; Wu, Wenjian; Wang, Yong; Wu, Minghong; Liu, Hao; Wang, Guoxiu

doi:10.1002/smtd.201900159

Cited by 224 publications

(138 citation statements)

References 199 publications

Supporting

Mentioning

137

Contrasting

Unclassified

Order By: Relevance

“…Nevertheless, achieving high content doping of SAMs in MOFs‐derived carbon is still a great challenge. [ 26–29 ] Low loading‐content severely hinders its practical use in current application fields [ 11–13 ] and also blocks its expansion in other fields such as SIBs. It is urgent to explore novel MOF‐derived stategies to realize high‐loading SAMs.…”

Section: Figurementioning

confidence: 99%

Carbon‐Microcuboid‐Supported Phosphorus‐Coordinated Single Atomic Copper with Ultrahigh Content and Its Abnormal Modification to Na Storage Behaviors

Kong

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

as N, B, O, S, and P, has been regarded as one of the most effective methods to boost the Na-ion storage in carbons by creating additional active sites and modifying the electronic structure of carbon. [6] Compared with nonmetal doping, doping of single atomic metal (SAM) is expected to exhibit more promising properties. Theoretical studies have shown that SAM dopants in graphene, such as Be-doped graphene, [7] Be,N dual-doped graphene, [8] and Si,Gecodoped graphene, [9] can enhance diffusion kinetics and provide anchoring sites for alkali metal-ions. SAM doping results in more delocalized electrons than nonmetal doping, enhancing electron conductivity. Additionally, SAMs render stronger affinity and lower migration resistance of alkali metal-ions in carbons. [10] Recent reports show that carbon-supported SAMs not only are being intensively investigated in electrocatalysts, [11] but also arouse great interests in Li-metal batteries [12] and Na-S batteries. [13] However, there is still no experimental investigation about the influence of SAMs on the Na-ion storage as well as other alkali metal-ion storage.Novel methods, such as atomic layer loading, chemical vapor deposition, wet chemistry route, and high-energy ball milling strategy, have been developed to prepare SAM-doped carbons, but they suffer from high cost and low yield. [11,14] Compared with these methods, metal-organic frameworks (MOFs)-derived strategy have gained tremendous popularity to construct carbonsupported SAMs. This method generally involves preparation of MOFs and subsequent pyrolysis. During pyrolysis, metal is exceedingly vulnerable to aggregate, [15] so maintaining single atomic state is a major challenge. Many strategies have been adopted to inhibit metal aggregation such as Zn-evaporation, [16][17][18][19][20][21][22] trapping of uncoordinated groups, [23][24][25] etc. Basic ideas for these methods are to increase the distance between metal atoms and/ or strengthen the interaction between metal and anchoring sites to avoid aggregation. Nevertheless, achieving high content doping of SAMs in MOFs-derived carbon is still a great challenge. [26][27][28][29] Low loading-content severely hinders its practical use in current application fields [11][12][13] and also blocks its expansion in other fields such as SIBs. It is urgent to explore novel MOF-derived stategies to realize high-loading SAMs.Achieving high-content loading of SAMs necessitates enhancing metal-ligand interaction. The MOF precursors for Carbon-supported single atomic metals (SAMs) have aroused great interest in energy conversion and storage fields. However, metal content has to date, been far below expectation. Additionally, theoretical calculations show that SAMs are superb anchoring sites for alkali metal-ion storage, but the experimental research remains untouched. Herein, a metal-organophosphine framework derived strategy is proposed to prepare carbon microcuboidssupported single atomic Cu with a high content of 26.3 wt%. Atomic Cu is stabilized mainly by P moieties, exhibit...

show abstract

Section: Figurementioning

confidence: 99%

Carbon‐Microcuboid‐Supported Phosphorus‐Coordinated Single Atomic Copper with Ultrahigh Content and Its Abnormal Modification to Na Storage Behaviors

Kong

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

show abstract

“…which provides large possibilities to anchor and stabilize single atoms and mass transport during the electrochemical reaction. [35] In spite of the progress that has been made, it remains a great challenge to synthesize the ideal SAC for NERR due to the lack of an appropriate synthesis method. Alternately, density functional theory (DFT) calculations contribute to the evaluation of the activity of single atoms stabilized by the supports with a well-defined structure.…”

Section: Single-atom Catalystsmentioning

confidence: 99%

Single-atom catalysts boost nitrogen electroreduction reaction

Zhai

Zhu

et al. 2020

Materials Today

View full text Add to dashboard Cite

Ammonia (NH3) is mainly produced through the traditional Haber-Bosch process under harsh conditions with huge energy consumption and massive carbon dioxide (CO2) emission. The nitrogen electroreduction reaction (NERR), as an energy-efficient and environment-friendly process of converting nitrogen (N2) to NH3 under ambient conditions, has been regarded as a promising alternative to the Haber-Bosch process and has received enormous interest in recent years. Although some exciting progress has been made, considerable scientific and technical challenges still exist in improving the NH3 yield rate and Faradic efficiency, understanding the mechanism of the reaction and promoting the wide commercialization of NERR. Single-atom catalysts (SACs) have emerged as promising catalysts because of its atomically dispersed activity sites and maximized atom efficiency, unsaturated coordination environment, and its unique electronic structure, which could significantly improve the rate of reaction and yield rate of NH3. In this review we briefly introduce the unique structural and electronic features of SACs, which contributes to comprehensively understand the reaction mechanism owing to their structural simplicity and diversity, and in turn expedite the rational design of fantastic catalysts at the atomic scale. Then, we summarize the most recent experimental and computational efforts on developing novel SACs with excellent NERR performance, including precious metal-, nonprecious metal-and nonmetal-based SACs. Finally, we present challenges and perspectives of SACs on NERR, as well as some potential means for advanced NERR catalyst.

show abstract

“…As summarized in some excellent review articles, SACs have been prepared mainly by two typical synthesis strategies, i.e., i) mass‐selected soft loading and atomic layer deposition; and ii) traditional wet‐chemistry methods. The characterization of SACs depends on some modern atomic‐resolution techniques .…”

Section: Sacs For Water Oxidationmentioning

confidence: 99%

Catalysis of a Single Transition Metal Site for Water Oxidation: From Mononuclear Molecules to Single Atoms

et al. 2019

View full text Add to dashboard Cite

The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201904037.Low-cost, nonprecious transition metal (TM) catalysts toward efficient water oxidation are of critical importance to future sustainable energy technologies. The advances in structure engineering of water oxidation catalysts (WOCs) with single TM centers as active sites, for example, single metallic molecular complexes (SMMCs), supported SMMCs, and single-atom catalysts (SACs) in recent reports are examined. The efforts made on these configurations in terms of design principle, advanced characterization, performances and theoretical studies, are critically reviewed. A clear roadmap with the correlations between the single-TM-site-based structures (coordination and geometric structure, TM species, support), and the catalytic performances in water oxidation is provided. The insights bridging SMMCs with SACs are also given. Finally, the challenges and opportunities in the single-TM-site catalysis are proposed.

show abstract

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

Cited by 224 publications

References 199 publications

Carbon‐Microcuboid‐Supported Phosphorus‐Coordinated Single Atomic Copper with Ultrahigh Content and Its Abnormal Modification to Na Storage Behaviors

Carbon‐Microcuboid‐Supported Phosphorus‐Coordinated Single Atomic Copper with Ultrahigh Content and Its Abnormal Modification to Na Storage Behaviors

Single-atom catalysts boost nitrogen electroreduction reaction

Catalysis of a Single Transition Metal Site for Water Oxidation: From Mononuclear Molecules to Single Atoms

Contact Info

Product

Resources

About