Metal‐Free Nitrogen Fixation at Boron

Hering‐Junghans, Christian

doi:10.1002/anie.201802675

Cited by 87 publications

(58 citation statements)

References 30 publications

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“…In contrast with N‐doped carbon materials, B doping leads to the polarization of the BC σ‐bond and induces a positive charge on the boron atom owing to the lower electronegativity of boron (2.04) as compared to that of carbon (2.55). Moreover, since N 2 is a weak Lewis base, it is sufficient to generate a Lewis acid electrocatalytic site with an unoccupied orbital by boron doping to bind N 2 (Figure b) . Based on this rationale, a pure B 4 C compound was prepared that ultimately gave an impressive yield of ammonia and high Faradaic efficiency .…”

Section: Design Principles For Electrocatalystsmentioning

confidence: 99%

“…Moreover, since N 2 is a weak Lewis base, it is sufficient to generate a Lewis acid electrocatalytic site with an unoccupied orbital by boron doping to bind N 2 (Figure 4b). [42,75] Based on this rationale, a pure B 4 C compound was prepared that ultimately gave an impressive yield of ammonia and high Faradaic efficiency. [76] It is known that the acceptance (back donation) of electrons in boron-based carbon electrocatalysts contributes to the activation of inert NN triple bonds.…”

Section: Atom Regulation In Metal-free Materialsmentioning

confidence: 99%

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

et al. 2020

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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.

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Section: Design Principles For Electrocatalystsmentioning

confidence: 99%

Section: Atom Regulation In Metal-free Materialsmentioning

confidence: 99%

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

et al. 2020

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“…In 2018, Hering-Junghans reported that hypovalent B species with the coexistence of lone-pair electrons and empty orbitals are similar to transition metals. [36] When doped into carbon materials, the B atoms could be positively charged and provided empty orbitals. Based on the Lewis theory that N 2 is a weak Lewis base, fabricating Lewis acid sites (empty orbitals of B) is considered to be a favorable strategy to realize the N 2 www.advancedsciencenews.com adsorption.…”

Section: Nonmetal Dopingmentioning

confidence: 99%

“…The most widely employed nonmetal‐atom dopant is boron (B) atom. In 2018, Hering‐Junghans reported that hypovalent B species with the coexistence of lone‐pair electrons and empty orbitals are similar to transition metals . When doped into carbon materials, the B atoms could be positively charged and provided empty orbitals.…”

Section: Defect Engineeringmentioning

confidence: 99%

Atomic Structure Modification for Electrochemical Nitrogen Reduction to Ammonia

Chen

Guo

et al. 2019

Advanced Energy Materials

128

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The electrochemical nitrogen reduction reaction (NRR), as an environmentally friendly method to convert nitrogen to ammonia at ambient temperature and pressure, has attracted the attention of numerous researchers. However, when compared with industrial production, electrochemical NRR often suffers from unsatisfactory yields and poor Faraday efficiency (FE). Recently, various structure engineering strategies have aimed to introduce extra active sites or enhance intrinsic activity to optimize the activation and hydrogenation of N2. In this review, recent progress in atomic structure modification is summarized and discussed to design high‐efficiency NRR catalysts, with a focus on defect engineering (heteroatom doping and atom vacancy), surface orientation and amorphization, as well as heterostructure engineering. In addition, existing challenges and future development directions are proposed to obtain more credible NRR catalysts with high catalytic performance and selectivity.

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“…1a), making many of them surprisingly stable under inert conditions. [1][2][3][4] Recently, transient dicoordinate (CAAC)-stabilised borylenes have drawn particular attention as compounds capable of activating and catenating N 2 , [21][22][23][24][25] the latter reaction being unprecedented even in transition metal chemistry.…”

Section: Introductionmentioning

confidence: 99%