MBenes: emerging 2D materials as efficient electrocatalysts for the nitrogen reduction reaction

Yang, Xiaowei; Shang, Chanjuan; Zhao, Jijun

doi:10.1039/d0nh00242a

Cited by 133 publications

(102 citation statements)

References 60 publications

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“…Although some MBene compounds have not yet been synthesized experimentally, theoretical predictions have verified that some MBenes can be electrochemical catalysts by theoretical studies. [ 16 ] Therefore, a large number of theoretical studies have reported that Pt(100) is suitable for the reaction of NO reduction to NH 3 , which is more difficult than N 2 and N 2 O formation. [ 17 ] However, NORR studies are mainly focused on metal‐based catalysts and single atom catalysts, but these catalysts usually face poor stability and require a high working potential during the NORR process.…”

Section: Introductionmentioning

confidence: 99%

Transition‐Metal Borides (MBenes) as New High‐Efficiency Catalysts for Nitric Oxide Electroreduction to Ammonia by a High‐Throughput Approach

Xiao

Chen

2021

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Here, the authors performed density functional theory calculations to study the catalytic performance of the nitric oxide reduction reaction (NORR) via a series of transition metal borides (MBenes). This work screened the M2B2 type MBenes from the IVB to V transition metals from the periodic table and systematically probed the catalytic activity and selectivity for the NORR process. It has been reported that Fe2B2, Mn2B2, and Rh2B2 can be high‐performance catalysts for converting NO to NH3 with smaller limiting potentials than other MBenes, and Nb2B2 and Hf2B2 have low limiting potentials of −0.11 V and −0.17 V for the NO production of NH3. The binding energy of ΔG*N can be a good descriptor of catalytic performance and is determined by the volcano plot of the rate‐determining step. The reaction mechanisms for NO reduction to NH3, N2, and N2O have been studied in detail, atomic *N can interact with another *N or one *NO molecule to form N2 and N2O via two successive hydrogenations. In this regard, *NO hydrogenation to *NOH has a lower formation energy than *HNO, and the MBenes have high selectivity for promoting the NORR and suppressing the hydrogen evolution reaction competition process.

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Section: Introductionmentioning

confidence: 99%

Transition‐Metal Borides (MBenes) as New High‐Efficiency Catalysts for Nitric Oxide Electroreduction to Ammonia by a High‐Throughput Approach

Xiao

Chen

2021

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“…[ 22 ] In particular, the abundant metal atoms distributed in basal plane can potentially provide partially occupied d orbitals to enhance the adsorption of small molecules, such as N 2 and other reaction intermediates, in the NRR process. [ 23 ] We note that, though the activity of several MBenes have been recently evaluated, [ 24 ] a large composition space of MBenes awaits explorations. [ 25 ] To achieve a rational design of optimal configuration toward NRR, it is important to identify the characteristics of the active sites, and to find out the suitable descriptors to evaluate their catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Establishing a Theoretical Landscape for Identifying Basal Plane Active 2D Metal Borides (MBenes) toward Nitrogen Electroreduction

Guo

Lin

et al. 2020

Adv Funct Materials

121

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To achieve efficient ammonia synthesis via electrochemical nitrogen reduction reaction (NRR), a qualified catalyst should have both high specific activity and large active surface area. However, integrating these two merits into one single material remains a big challenge due to the difficulty in balancing multiple reaction intermediates. Here, it is demonstrated that the boron‐analogues of MXenes, namely “MBenes”, could cope with the challenge and achieve the high activity and large reaction region simultaneously toward NRR. Using extensive density functional theory computations and taking 16 MBenes as representatives, it is identified that seven MBenes (CrB, MoB, WB, Mo2B, V3B4, CrMnB2, and CrFeB2) not only have intrinsic basal plane activity for NRR with limiting potentials ranging from −0.22 to −0.82 V, but also possess superior capability of suppressing the competitive hydrogen evolution reaction. Particularly, different from the MXenes whose surface oxidation may block the active sites, once oxidized, these MBenes can catalyze NRR via the self‐activating process, reducing O*/OH* into H2O* under reaction conditions, and favoring the N2 electroreduction. As a result, the exceptional activity and selectivity, high active area (≈1019 m−2), and antioxidation nature render these MBenes as pH‐universal catalysts for NH3 production without introducing any dopants and defects.

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“…Thus, the limiting potential (η) of NRR on Fe 3 @C 2 N is as low as −0.57 V, lower than the η values on the Ru (0001) step surface [40] and Fe 2 @C 2 N [24] (0.98 eV and 1.23 eV, respectively). Typically, the potential limiting step on most metal surfaces (such as Re, Ru, Rh and Fe) or two-dimensional MBenes is either the first hydrogenation (forming *NNH) or the last protonation (*NH 3 formation or NH 3 desorption) [9,41]. However, on Fe 3 @C 2 N, the free energy change of *N 2 → *NNH is only 0.28 eV.…”

Section: N 2 Reaction On Fe 3 @C 2 Nmentioning

confidence: 99%

Fe3 Cluster Anchored on the C2N Monolayer for Efficient Electrochemical Nitrogen Fixation

Han

Meng

et al. 2020

Catalysts

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Under the current double challenge of energy and the environment, an effective nitrogen reduction reaction (NRR) has become a very urgent need. However, the largest production of ammonia gas today is carried out by the Haber–Bosch process, which has many disadvantages, among which energy consumption and air pollution are typical. As the best alternative procedure, electrochemistry has received extensive attention. In this paper, a catalyst loaded with Fe3 clusters on the two-dimensional material C2N (Fe3@C2N) is proposed to achieve effective electrochemical NRR, and our first-principles calculations reveal that the stable Fe3@C2N exhibits excellent catalytic performance for electrochemical nitrogen fixation with a limiting potential of 0.57 eV, while also suppressing the major competing hydrogen evolution reaction. Our findings will open a new door for the development of non-precious single-cluster catalysts for effective nitrogen reduction reactions.

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MBenes: emerging 2D materials as efficient electrocatalysts for the nitrogen reduction reaction

Abstract: MBenes hold many merits for electrocatalysis of the nitrogen reduction reaction, including outstanding stability in aqueous environments, excellent electrical conductivity, an inhibited hydrogen evolution reaction, and highly active boron and metal surfaces.

Cited by 133 publications

References 60 publications

Transition‐Metal Borides (MBenes) as New High‐Efficiency Catalysts for Nitric Oxide Electroreduction to Ammonia by a High‐Throughput Approach

Transition‐Metal Borides (MBenes) as New High‐Efficiency Catalysts for Nitric Oxide Electroreduction to Ammonia by a High‐Throughput Approach

Establishing a Theoretical Landscape for Identifying Basal Plane Active 2D Metal Borides (MBenes) toward Nitrogen Electroreduction

Fe3 Cluster Anchored on the C2N Monolayer for Efficient Electrochemical Nitrogen Fixation

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