Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries

Qiu, Hua‐Jun; Du, Peng; Hu, Kailong; Gao, Jiaojiao; Li, Huanglong; Chen, Mingwei; Ina, Toshiaki; Ohara, Koji; Ito, Yoshikazu; Chen, Ming-Wei

doi:10.1002/adma.201900843

Cited by 259 publications

(145 citation statements)

References 71 publications

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“…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

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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...

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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

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“…Other Transitional Metal Single‐Atom Catalysts : A 3D nanoporous graphene (np‐graphene) doped with both N and Ni single atoms/clusters was reported, which used CVD method to predope N and then facilitated the anchoring of Ni. [ 175 ] In the codoped graphene, the atomic percentage of nitrogen was detected to be about 3 at% and the loading of Ni could reach as high as ≈23 wt%, including clusters and isolated atoms. The final product was proved to form NiN and NiC bonding which indicated atomic Ni dispersion ( Figure a–d).…”

Section: Application In Advanced Battery Systemsmentioning

confidence: 99%

Single‐Atom Catalytic Materials for Advanced Battery Systems

2020

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power and energy densities are the imperative units for these cutting-edge energy harvesting and storage. [3] The state-ofthe-art commercial batteries are prepared with graphite anodes and lithium transition-metal oxide cathodes that reversibly intercalate lithium (Li) ions with moderate stability and energy densities. [4] The intrinsic physicochemical properties and ion insertion mechanisms of conventional materials limits the energy capacity of devices, which will not be quantified for unprecedented demand of modern electronics. [5] Other than the insertiontype electrode materials, there exist some conversion-type electrode materials with higher energy storage capability and faster electrochemical conversion dynamics, including transition-metal dichalcogenide (TMD) and silicon materials. [6] TMD materials demonstrate strong chemical interaction and high catalytic effect with active species in batteries, which is critical to suppress shuttle effects and promote conversion kinetics. [7] But lithiation of TMD materials inevitably gives rise to phase transformation and causes severe damage for the structural integrity of electrodes. [8] Silicon materials emerge as promising conversion-type substitute in recent years due to the high theoretical capacity of 4200 mAh g −1 , but silicon materials exit severe volume expansion effect in conversion processes, which will lead to rapid capacity degradation within several cycles. [9] These two typical conversion-type materials are both semiconductor materials with poor conductivity and unsatisfactory structural stability under electrochemical conditions. Construction of composition architectures with carbon materials is a common strategy to address these drawbacks for purpose of increasing conductivity and maintaining structural integrity. [10] Even if some synthetic methods have been deliberately considered and rationally designed, their attractive theoretical capacities have not fully expressed with long-term cycling performances. Thus, novel battery chemistries other than traditional insertion and conversion-type electrode materials need to be developed to address these issues.With the ever-increasing development of material science and engineering, lots of alternative materials with high energy capacities and stabilities have stood out as the electrode materials from the competition with conventional counterparts. For instance, sulfur material-based batteries gives high theoretical Advanced battery systems with high energy density have attracted enormous research enthusiasm with potential for portable electronics, electrical vehicles, and grid-scale systems. To enhance the performance of conversiontype batteries, various catalytic materials are developed, including metals and transition-metal dichalcogenides (TMDs). Metals are highly conductive with catalytic effects, but bulk structures with low surface area result in low atom utilization, and high chemical reactivity induces unfavorable dendrite effects. TMDs present chemical adsorption with active species and ...

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“…Disappointingly, single precious noble metal catalysts (PNMCs) generally are not sufficient since they are not simultaneously providing enough activity for both ORR and OER, and they suffer from the scarcity and electrochemical instability . Therefore, it is critical to develop nonprecious metal catalysts (NPMCs) with high bifunctional activity, low cost and superior stability …”

Section: Introductionmentioning

confidence: 99%

“…[12] Therefore, it is critical to develop nonprecious metal catalysts (NPMCs) with high bifunctional activity,low cost and superior stability. [13] Emerging as ac lass of outstanding alternatives, the transition-metal (Fe, Co, Ni, etc.) andt heir derivativesh ave attracted great attention recently as bifunctional oxygen electrocatalysts.…”

Section: Introductionmentioning

confidence: 99%

The Proportion of Fe‐N_X, N Doping Species and Fe₃C to Oxygen Catalytic Activity in Core‐Shell Fe‐N/C Electrocatalyst

Liu

Zhu

Jiang

et al. 2019

Chemistry An Asian Journal

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Ab ifunctional oxygen electrocatalyst composed of iron carbide( Fe 3 C) nanoparticles encapsulatedb yn itrogen doped carbon sheetsi sr eported. X-ray photoelectron spectroscopy and X-ray absorption neare dge structure revealed the presence of severalk inds of active sites (FeÀN x sites, N doping sites) and the modulated electron structure of nitrogen doped carbon sheets. Fe 3 C@N-CSs shows excellent oxygen evolution and oxygen reduction catalytic activity owing to the modulated electron structure by encapsulated Fe 3 Cc orev ia biphasic interfaces electron interaction, which can lower the free energy of intermediate, strengthen the bondings trength and enhance conductivity.M eanwhile, the contribution of the FeÀN x sites, Nd oping sites and the effect of Fe 3 Cc ore for the electrocatalytic oxygen reaction is originally revealed. The Fe 3 C@N-CSsa ir electrode-based zincair battery demonstrates ah igh open circuit potentialo f 1.47 V, superior charge-discharge performance and long lifetime, which outperforms the noble metal-based zinc-air battery.

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Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries

Cited by 259 publications

References 71 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 Catalytic Materials for Advanced Battery Systems

The Proportion of Fe‐N_X, N Doping Species and Fe₃C to Oxygen Catalytic Activity in Core‐Shell Fe‐N/C Electrocatalyst

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Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries

Cited by 259 publications

References 71 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 Catalytic Materials for Advanced Battery Systems

The Proportion of Fe‐NX, N Doping Species and Fe3C to Oxygen Catalytic Activity in Core‐Shell Fe‐N/C Electrocatalyst

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The Proportion of Fe‐N_X, N Doping Species and Fe₃C to Oxygen Catalytic Activity in Core‐Shell Fe‐N/C Electrocatalyst