Metal-free boron carbonitride with tunable boron Lewis acid sites for enhanced nitrogen electroreduction to ammonia

Chang, Bin; Li, Lili; Shi, Danni; Jiang, Huaidong; Ai, Zizheng; Wang, Shouzhi; Shao, Yongliang; Shen, Jianxing; Wu, Yongzhong; Li, Yanlu; Hao, Xiaopeng

doi:10.1016/j.apcatb.2020.119622

Cited by 129 publications

(63 citation statements)

References 58 publications

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“…Since nitrogen is a weak Lewis base, the NN triple bond can be activated by a Lewis acid site with an empty orbital to accept lone pair electrons of nitrogen . Therefore, the formation of abundant Lewis acid sites is beneficial for the improvement of nitrogen reduction performance.…”

Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Wen

Zhang

et al. 2021

ACS Appl. Mater. Interfaces

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Introducing oxygen vacancy (V o ) has been considered as an effective and significant method to accelerate the sluggish electrocatalytic nitrogen reduction reaction (NRR). In this work, a series of bimetallic zeolitic imidazolate frameworks based on ZIF-67 and ZIF-8 with varied ratios of Co/Zn have been applied as precursors to prepare V o -rich Zn-doped Co 3 O 4 nanopolyhedrons (Zn−Co 3 O 4 ) by a low-temperature oxidation strategy. Zn−Co 3 O 4 presents an ammonia yield of 22.71 μg h −1 mg cat.−1 with a high faradaic efficiency of 11.9% for NRR under ambient conditions. The remarkable catalytic performances are believed to result from the plentiful V o as the Lewis acid sites and electron-rich Co sites to promote the adsorption and dissociation of N 2 molecules. Remarkably, Zn−Co 3 O 4 also demonstrates a high electrochemical stability. This work presents a guiding method for developing a stable and efficient electrocatalyst for the NRR.

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Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Wen

Zhang

et al. 2021

ACS Appl. Mater. Interfaces

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“…In addition, two smaller peaks can also be observed, which correspond to the CF semi‐ionic bond (290.3 eV) and the CF covalent bond (291.3 eV). [ 19,38 ] The N 1 s spectrum shown in Figure 3c can be fit to four peaks corresponding to graphite N‐bonds (NQ) (401.7 eV), pyrrole N‐bonds (N‐5) (399.8 eV), and pyridine N‐bonds (N‐6) (398.6 eV) and B‐N bonds (397.9 eV). The contents of N5 and N6 increased after the incorporation of F, compared with BCN as shown in the N 1 s spectrum in Figures 3c and S2d, Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

“…The specific capacity of the BCN material based on the contribution of the electric double layer needs to be further improved. [ 4,19,20 ] Research on fluorine‐doped supercapacitor materials is still insufficient in the present stage due to the hydrophobic nature of the fluorine functional group. However, doping F in graphene electrode materials can promote charge redistribution between adjacent carbon atoms, resulting in high electronegativity and effectively improving the electrochemical activity and stability of graphene.…”

Section: Introductionmentioning

confidence: 99%

Self‐Supported Fluorine‐Doped Boron Carbonitride Porous Aerogels for High‐Performance Supercapacitors

Liu

Shi

et al. 2021

Energy Tech

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Carbon materials have long been extensively used in supercapacitors. However, the practical application of carbon‐based supercapacitors has been severely limited by their low charge storage capacity. Rational construction of carbon materials with heteroatom doping and high specific surface area can effectively improve the performance of supercapacitors. Therefore, a self‐supported fluorine‐doped boron carbonitride (F‐BCN) aerogel material for the application of supercapacitors is designed. The introduction of heteroatoms increases the defect density of the carbon skeleton, expands the interlayer spacing, and generates abundant electrochemical active sites, thereby promoting the diffusion of ions in the electrode. The specific capacitance of F‐BCN‐3 is 524.9 F g−1 at a specific current of 1 A g−1, with which the assembled symmetric supercapacitor exhibits a maximum energy density of 11.75 W h kg−1. The symmetric supercapacitor can maintain a specific capacitance of 83% after 5000 charge and discharge cycles, showing good electrochemical cycle stability. The design concept provides a promising guide for further applications of carbon materials in energy storage devices.

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“…It is worth noting that boron carbonitride (BCN) has recently been proved to be an effective electrocatalytic catalyst with excellent stability [ 97 , 98 ]. Taking representative research as an example, Lewis acid–base theory and DFT revealed that the enrichment of B/N heteroatoms in boron carbon nitride (BCN) system could lead to stronger OH*/H 2 O adsorption strength, respectively [ 98 ].…”

Section: Electrocatalytic Performance Of Anion-mixed Electrocatalystsmentioning

confidence: 99%

Shining Light on Anion-Mixed Nanocatalysts for Efficient Water Electrolysis: Fundamentals, Progress, and Perspectives

et al. 2022

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Highlights This review introduces recent advances of various anion-mixed transition metal compounds (e.g., nitrides, halides, phosphides, chalcogenides, (oxy)hydroxides, and borides) for efficient water electrolysis applications in detail. The challenges and future perspectives are proposed and analyzed for the anion-mixed water dissociation catalysts, including polyanion-mixed and metal-free catalyst, progressive synthesis strategies, advanced in situ characterizations, and atomic level structure–activity relationship. Abstract Hydrogen with high energy density and zero carbon emission is widely acknowledged as the most promising candidate toward world's carbon neutrality and future sustainable eco-society. Water-splitting is a constructive technology for unpolluted and high-purity H2 production, and a series of non-precious electrocatalysts have been developed over the past decade. To further improve the catalytic activities, metal doping is always adopted to modulate the 3d-electronic configuration and electron-donating/accepting (e-DA) properties, while for anion doping, the electronegativity variations among different non-metal elements would also bring some potential in the modulations of e-DA and metal valence for tuning the performances. In this review, we summarize the recent developments of the many different anion-mixed transition metal compounds (e.g., nitrides, halides, phosphides, chalcogenides, oxyhydroxides, and borides/borates) for efficient water electrolysis applications. First, we have introduced the general information of water-splitting and the description of anion-mixed electrocatalysts and highlighted their complementary functions of mixed anions. Furthermore, some latest advances of anion-mixed compounds are also categorized for hydrogen and oxygen evolution electrocatalysis. The rationales behind their enhanced electrochemical performances are discussed. Last but not least, the challenges and future perspectives are briefly proposed for the anion-mixed water dissociation catalysts.

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Metal-free boron carbonitride with tunable boron Lewis acid sites for enhanced nitrogen electroreduction to ammonia

Cited by 129 publications

References 58 publications

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Self‐Supported Fluorine‐Doped Boron Carbonitride Porous Aerogels for High‐Performance Supercapacitors

Shining Light on Anion-Mixed Nanocatalysts for Efficient Water Electrolysis: Fundamentals, Progress, and Perspectives

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Metal-free boron carbonitride with tunable boron Lewis acid sites for enhanced nitrogen electroreduction to ammonia

Cited by 129 publications

References 58 publications

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co3O4 Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co3O4 Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Self‐Supported Fluorine‐Doped Boron Carbonitride Porous Aerogels for High‐Performance Supercapacitors

Shining Light on Anion-Mixed Nanocatalysts for Efficient Water Electrolysis: Fundamentals, Progress, and Perspectives

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Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation

Oxygen Vacancy Engineering of MOF-Derived Zn-Doped Co₃O₄ Nanopolyhedrons for Enhanced Electrochemical Nitrogen Fixation