Rational Design of Fe–N/C Hybrid for Enhanced Nitrogen Reduction Electrocatalysis under Ambient Conditions in Aqueous Solution

Wang, Ying; Cui, Xiaoqiang; Zhao, Jingxiang; Jia, Guangri; Gu, Lin; Zhang, Qinghua; Meng, Lingkun; Shi, Zhan; Zheng, Lirong; Wang, Chunyu; Zhang, Ziwei; Zheng, Weitao

doi:10.1021/acscatal.8b03802

Cited by 304 publications

(210 citation statements)

References 75 publications

Supporting

Mentioning

199

Contrasting

Order By: Relevance

“…PGM‐free SACs, including Mo and Fe based electrocatalysts, have also been studied for the NRR. In particular, the FeN 4 catalyst exhibited an NH 3 yield rate of 62.9 ± 2.7 µg h −1 mg−1 cat.…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis Formentioning

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

293

240

View full text Add to dashboard Cite

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.

show abstract

Section: Atomically Dispersed Single Metal Site Electrocatalysis Formentioning

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

293

240

View full text Add to dashboard Cite

show abstract

“…Based on N 2 temperature‐programmed desorption and DFT calculation, the author revealed that the coordination of Ru with N atom can enhance the adsorption energy for N 2 molecule, thus improving the reaction activity. Except the noble‐atom SACs, the Mo and Fe based SACs have recently been studied for electrocatalytic NRR and exhibit competitive activities.…”

Section: Electrocatalytic Performancementioning

confidence: 99%

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Zhu

Peng

et al. 2019

Small Methods

View full text Add to dashboard Cite

Single‐atom catalysts (SACs) on 2D nanomaterials have great potential as efficient and low‐cost electrocatalysts for clean energy technologies. The coordination environments, as well as the physicochemical properties of the 2D supports, play key roles in tuning the catalytic activity and reaction mechanism of the single‐atom centers. This review first summarizes the suitable synthetic strategies of single‐atom on different 2D supports. The methods that facilitate the formation of relative homogeneous structure and enable the regulation of the surrounding atomic environment of metal center are discussed. Furthermore, the recent progress of SACs for energy‐related electrochemical applications is reviewed, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. The strategies about modulation of the electronic structure of single‐atom for enhanced performance are highlighted, together with a discussion of the current issues and the prospects of this field.

show abstract

“…A typical example is the metal–organic framework compound‐carbon nanotube (MOF‐CNT)‐derived Fe−N/C electrocatalyst. When NRR took place on Fe−N/C with built‐in Fe−N 3 active sites, all of the features, including the hierarchically porous architecture together with large surface area, positively charged surface, and weak ferromagnetism, contributed to NRR activity . Computational study of single‐atom Fe revealed that increasing the magnetic moment strengthened the adsorption of dinitrogen and promoted charge transfer from graphene substrate to the adsorbed dinitrogen molecule .…”

Section: Design Principles For Electrocatalystsmentioning

confidence: 99%

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

et al. 2020

View full text Add to dashboard Cite

Ammonia (NH3) is a pivotal precursor in fertilizer production and a potential energy carrier. Currently, ammonia production worldwide relies on the traditional Haber–Bosch process, which consumes massive energy and has a large carbon footprint. Recently, electrochemical dinitrogen reduction to ammonia under ambient conditions has attracted considerable interest owing to its advantages of flexibility and environmental friendliness. However, the biggest challenge in dinitrogen electroreduction, i.e., the low efficiency and selectivity caused by poor specificity of electrocatalysts/electrolytic systems, still needs to be overcome. Although substantial progress has been made in recent years, acquiring most available electrocatalysts still relies on low efficiency trial‐and‐error methods. It is thus imperative to establish some critical guiding principles for nitrogen electroreduction toward a rational design and accelerated development of this field. Herein, a basic understanding of dinitrogen electroreduction processes and the inherent relationships between adsorbates and catalysts from fundamental theory are described, followed by an outline of the crucial principles for designing efficient electrocatalysts/electrocatalytic systems derived from a systematic evaluation of the latest significant achievements. Finally, the future research directions and prospects of this field are given, with a special emphasis on the opportunities available by following the guiding principles.

show abstract

Rational Design of Fe–N/C Hybrid for Enhanced Nitrogen Reduction Electrocatalysis under Ambient Conditions in Aqueous Solution

Cited by 304 publications

References 75 publications

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

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

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

Contact Info

Product

Resources

About