Electrochemical Nitrogen Reduction Reaction Performance of Single-Boron Catalysts Tuned by MXene Substrates

Zheng, Shu Guo; Li, Shunning; Mei, Zongwei; Hu, Zongxiang; Chu, Mihai; Liu, Jiahua; Chen, Xin; Pan, Feng

doi:10.1021/acs.jpclett.9b02741

Cited by 133 publications

(86 citation statements)

References 64 publications

(102 reference statements)

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“…SACs with other single-atom centers (Fe, Co, Mo, B, etc.) have also been investigated in NRR (172)(173)(174)(175)(176)(177)(178)(179)(180). For instance, Ou et al (181) systematically studied the Gibbs free energies for *H (G* H ) and *N 2 (G* N2 ) on various Mo-based SACs.…”

Section: Nitrogen Reduction Reactionmentioning

confidence: 99%

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Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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Section: Nitrogen Reduction Reactionmentioning

confidence: 99%

“…SACs with other single-atom centers (Fe, Co, Mo, B, etc.) have also been investigated in NRR ( 172 – 180 ). For instance, Ou et al .…”

Section: Nitrogen Reduction Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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“…MXene, an emerging typical 2D material, can be expressed by the chemical formula of M n +1 X n T x ( n = 1, 2 and 3), [ 18,20 ] where M stands for the transition metal (e.g., Ti, Ta, Nb, V, Mo), the X represents the nitrogen or carbon or carbonitride, while T x represents a large number of surface functional groups (e.g., OH, F). [ 21,22 ] Due to the excellent conductivity and stability, Ti 3 C 2 T x MXenes have been demonstrated by several theoretical calculations [ 20,22 ] and experimental results [ 5,23–26 ] as promising NRR catalysts, with key performance summarized in Table S1, Supporting Information. To meet the requirement from the NH 3 industry, however, there is still a large gap to be filled prior to their practical applications, for both NH 3 yield and NRR selectivity.…”

Section: Figurementioning

confidence: 99%

“…Therefore, a basic guideline for further improvement is to increase Ti‐edge atoms, which could be achieved through reducing the MXene size, [ 23,25,26 ] thus MXene QDs should be an attractive candidate. Furthermore, MXene samples are often covered by surface functional groups, mainly including OH, F, and O, [ 21,22 ] inevitably formed during the synthesis, which can directly affect the catalysis performance. For instance, terminal oxygen on the basal planes is suggested to be essential to bridge over a high energy barrier to advance the NRR.…”

Section: Figurementioning

confidence: 99%

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Jin

Liu

et al. 2020

Advanced Energy Materials

165

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Ammonia (NH 3 ) is essential to human life due to its vital roles in fuel production, agricultural cultivation and industrial manufacture. [1,2] The abundant nitrogen (N 2 ) in the earth's atmosphere is the main raw material for the synthesis of NH 3 , [3] but the large bond energy (940.95 kJ mol −1 ) of NN bond [1,4] makes N 2 reduction reaction (NRR) extremely difficult. [5] At present, the traditionally industrial NH 3 synthesis strongly relies on the Haber-Bosch process, which has to be conducted at high pressures at 200-300 atm and high temperature of ≈500 °C. [6] Furthermore, such production method is energy-intensive that consumes 1-3% of the global energy annually and emit tons of CO 2 correspondingly. [7] Over the last decades, electrochemical NRR has attracted global attention due to its renewable raw materials of N 2 and water as well as ambient synthesis condition. [8] With recent booming development, the study of NRR electrocatalysts has moved from precious metals to cheap and abundant transition metal oxides and metal-free materials, etc. [9] However, due to the lack of rational and target-specific design of the NRR electrocatalyst, it is still a difficult task to reach an ideal electrocatalyst fulfilling with the requirements of high NH 3 yield, excellent selectivity and cost-effectiveness simultaneously. To meet these requirements, it is expected that catalysts contain abundant active sites. [10] Under this context, various low-dimensional catalysts have been extensively investigated, such as 2D nanosheets and 0D quantum dots (QDs) due to their ultrahigh ratio of active sites and defects exposed on the surfaces.QDs, especially derived from 2D materials (2D-QDs), are often with small size of less than 10 nm, enhanced surface defects and large surface specific area, thus offering abundantactive basal and edge sites, together with various functional groups. [8,11,12] As a result, a large space has been generated for advanced rational design for N 2 adsorption and full reduction. [13,17] So far, however, the effect of edge sites and their functional groups on NRR performance of 2D-QDs is poorly known. MXene, an emerging typical 2D material, can be expressed by the chemical formula of M n+1 X n T x (n = 1, 2 and 3), [18,20] where M stands for the transition metal (e.g., Ti, Ta, Nb, V, Mo), the X represents the nitrogen or carbon or carbonitride, while T x represents a large number of surface functional groups (e.g., OH, F). [21,22] Due to the excellent conductivity and stability, To enable an efficient and cost-effective electrocatalytic N 2 reduction reaction (NRR) the development of an electrocatalyst with a high NH 3 yield and good selectivity is required. In this work, Ti 3 C 2 T x MXene-derived quantum dots (Ti 3 C 2 T x QDs) with abundant active sites enable the development of efficient NRR electrocatalysts. Given surface functional groups play a key role on the electrocatalytic performance, density functional theory calculations are first conducted, clarifying that hydroxyl groups on Ti 3 C 2...

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“…Recently, it is proved that strong back-donation from boron (B) centers to N 2 can effectively realize N 2 reduction. Through DFT calculations, Zheng et al [84] systematically studied the catalytic performance of single B atoms decorated on 2D transition metal carbides (MXenes). The B-doped Mo 2 CO 2 and W 2 CO 2 MXenes have excellent catalytic activity and selectivity, and their limiting potentials are −0.20 and −0.24 V, respectively.…”

Section: Nitrogen Reduction Reactionmentioning

confidence: 99%

Recent Progress in MXene‐Based Materials: Potential High‐Performance Electrocatalysts

Liu

Liang

Ren

et al. 2020

Adv Funct Materials

219

144

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The family of transition metal carbides, nitrides, and carbonitrides (collectively called MXenes) has been a thriving field since the first invention of Ti3C2Tx (MXene) in 2011. MXene is a new type of nanometer 2D sheet material, which exhibits great application potentials in various fields due to its multiple advantages such as high specific surface area, good electrical conductivity, and high mechanical strength. Electrocatalysis is regarded as the core of future clean energy conversion technologies, and MXene‐based materials provide inspiration for the design and preparation of electrocatalysts with high activity, high selectivity, and long loading life time. The applications of MXene‐based materials in electrocatalysis, including hydrogen evolution reaction, nitrogen reduction reaction, oxygen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, and methanol oxidation reaction are summarized in this review. As a crucial session regarding experiments, the current safer and more environmentally friendly preparation methods of MXene are also discussed. Focusing on the materials design and enhancement methods, the key challenges and opportunities for MXene‐based materials as a next‐generation platform in both fundamental research and practical electrocatalysis applications are presented. This account serves to promote future efforts toward the development of MXenes and related materials in the electrocatalysis applications.

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Electrochemical Nitrogen Reduction Reaction Performance of Single-Boron Catalysts Tuned by MXene Substrates

Cited by 133 publications

References 64 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Recent Progress in MXene‐Based Materials: Potential High‐Performance Electrocatalysts

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Electrochemical Nitrogen Reduction Reaction Performance of Single-Boron Catalysts Tuned by MXene Substrates

Cited by 133 publications

References 64 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Rational Design of Hydroxyl‐Rich Ti3C2Tx MXene Quantum Dots for High‐Performance Electrochemical N2 Reduction

Recent Progress in MXene‐Based Materials: Potential High‐Performance Electrocatalysts

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Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction