The rational design of single-atom catalysts for electrochemical ammonia synthesis <i>via</i> a descriptor-based approach

Long, Jun; Fu, Xianliang; Xiao, Jianping

doi:10.1039/d0ta05943a

Cited by 63 publications

(51 citation statements)

References 48 publications

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“…It was first reported by Nørskov and co‐workers 20 that the adsorption energies for adsorbates (CH x , NH x , OH x , and SH x ) on different transition metal surfaces are correlated well. The scaling relation has been found over different kinds of materials too 8,19,43–44 . The adsorption energies over the surfaces (ZnO and Cu/ZnO) 45–46 with different oxygen vacancies are also correlated well.…”

Section: The General Scaling Relations Beyond Accuracy In Energeticsmentioning

confidence: 61%

“…The scaling relation has been found over different kinds of materials too. 8,19,[43][44] The adsorption energies over the surfaces (ZnO and Cu/ZnO) [45][46] with different oxygen vacancies are also correlated well. There is no doubt that the calculated adsorption energy should be affected by functionals, structure models, and corrections (e.g., solvent effect, van der Waals forces).…”

Section: The General Scaling Relations Beyond Accuracy In Energeticsmentioning

confidence: 75%

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Toward computational design of chemical reactions with reaction phase diagram

Guo

Long

et al. 2021

WIREs Comput Mol Sci

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Density functional theory (DFT) was rapidly developed and achieved a great success in the last decades. As the advancement of general concepts in heterogeneous catalysis, theoretical study of chemical reactions based on DFT calculations has become more and more feasible, which provides a guideline for the rational design of novel catalysts toward higher reaction activity and specific selectivity. Here, we review an innovate scheme, namely reaction phase diagram (RPD), which can offer not only an in-depth understanding of reaction mechanisms, but also the prediction of catalytic activity and selectivity trend over a collection of catalysts. The RPD analysis was successfully applied to understand the activity variation of CO 2 electroreduction to CO and formic acid, as well as thermochemical hydrogenation and dehydrogenation. Meanwhile, the RPD analysis also exhibits a success of studying the product selectivity in syngas conversion to methane, ethanol, and methanol with complicated reaction pathways. At the end, we review a successful case of catalyst rational design with a target of NO selective electroreduction to ammonia. The foundation of RPD analysis is based on the scaling relation of adsorption energies and the correlation between kinetic barriers and reaction energies at elementary steps. Therefore, microkinetic modeling is complementary to the RPD analysis. A few of limitations and the prospect of the development regarding the RPD analysis are addressed in this review. This article is categorized under:Structure and Mechanism > Reaction Mechanisms and Catalysisdensity functional theory, full pathway construction, global energy optimization, heterogeneous catalysis, reaction phase diagram | INTRODUCTIONHeterogeneous catalysis possesses a momentous value in many chemical processes, which has been widely focused in industry. Besides, it has been widely studied in academia, for example Fischer-Tropsch (FT) and ammonia synthesis, 1-3 selective catalytic reduction (SCR), CO oxidation, 4-5 CO 2 reduction reaction (CO 2 RR), and oxygen reduction reaction Chenxi Guo and Xiaoyan Fu contributed equally in this work.

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Section: The General Scaling Relations Beyond Accuracy In Energeticsmentioning

confidence: 61%

Section: The General Scaling Relations Beyond Accuracy In Energeticsmentioning

confidence: 75%

Toward computational design of chemical reactions with reaction phase diagram

Guo

Long

et al. 2021

WIREs Comput Mol Sci

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“…The corresponding adsorption Δ G of H 2 O and H + species are −0.50 and −0.64 eV, respectively, which are more positive than the Δ G

_{* normalN_{2}}

(−0.80 eV), indicating an adsorption preference for N 2 adsorption. According to previous reports, the U L of NRR [ U L (NRR)] of transition metal‐based catalysts are around −0.4 to −0.8 V for NRR [14,28,32,34,38,68–79] . Figure 4 shows the U L (NRR) and U L of HER [ U L (HER)] on various catalysts where the red symbols represent the electrocatalysts selective for HER, while blue ones are more favorable for NRR.…”

Section: Resultsmentioning

confidence: 71%

“…According to previous reports, the U L of NRR [U L (NRR)] of transition metal-based catalysts are around À 0.4 to À 0.8 V for NRR. [14,28,32,34,38,[68][69][70][71][72][73][74][75][76][77][78][79] Figure 4 shows the U L (NRR) and U L of HER [U L (HER)] on various catalysts where the red symbols represent the electrocatalysts selective for HER, while blue ones are more favorable for NRR. Particularly, the U L (NRR) on Os 1 B 11 N 12 /C 2 N is lower than that of previous reports.…”

Section: Resultsmentioning

confidence: 99%

Os₁B₁₁N₁₂/C₂N as an Efficient Electrocatalyst for Nitrogen Reduction Reaction

et al. 2022

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Ammonia is one of the most important fertilizer feedstocks and chemical precursor besides a promising hydrogen carrier. However, the electrochemical reduction of nitrogen to ammonia is impeded by the low selectivity and high limiting potential of reported catalysts. Herein, the nitrogen reduction reaction (NRR) on Os-doped BN cluster supported on C 2 N (Os 1 B 11 N 12 /C 2 N) was investigated systematically based on density functional theory calculations. It was found that the adjustment of BN cluster on the upper d-band edge of Os atom enabled the optimal adsorption strength for NRR intermediates. Consequently, Os 1 B 11 N 12 /C 2 N exhibited high catalytic activity for NRR with the limiting potential of À 0.34 V and a remarkable suppressive effect on the hydrogen evolution reaction. This work is not only beneficial for understanding the mechanism of NRR but also provides a fundamental guidance for rational design of catalysts for NRR.

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“…Rational design of SACs: Engineering the rational design for large-scale production of SACs is highly desirable for its key advancement in various fields. [347] Several theoretical [128,[348][349][350] and experimental models [351][352][353] are given for SACs rational designs. Besides these predictable models, understanding the catalytic activity and its composition relation is highly complex and challenging.…”

Section: Future Directions and Applicationsmentioning

confidence: 99%

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

Singh

Sharma

Gaikwad

et al. 2021

Small

146

106

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In order to achieve these goals, it is of fundamental importance to design new catalysts that enable new benign routes to produce/ store and convert renewable energies and to obtain chemicals from waste. [3][4][5] We need to design new chemical pathways that replace traditional petrochemicalbased routes, considering new platform molecules, possibly derived by renewable resources such as agriculture/municipal wastes. This transition must fully involve the energy sector, with the entire redefinition of the pool of energy vectors for transportations, building heating systems, and power production. As the burning of fossil fuels and biomass are not anymore compatible with the dramatic increasing air pollution and global warming.To achieve all these targets, we will need to design nontoxic, earth-abundant, and less-expensive, highly efficient, and selective catalysts that can work under mild reaction conditions without producing significant waste. [6,7] Catalytic activity and selectivity are enabled via the many factors such as accessibility of active sites, interaction with the surface, i.e., varying support and coordinating sphere, composition of metals (bimetallic and many-metallic), size and shape; and chemical states of active sites which can to tailored via developing 2D catalyst [8][9][10] or via developing single atomic sites stabilized on hollow A heterogeneous catalyst is a backbone of modern sustainable green industries; and understanding the relationship between its structure and properties is the key for its advancement. Recently, many upscaling synthesis strategies for the development of a variety of respectable control atomically precise heterogeneous catalysts are reported and explored for various important applications in catalysis for energy and environmental remediation. Precise atomic-scale control of catalysts has allowed to significantly increase activity, selectivity, and in some cases stability. This approach has proved to be relevant in various energy and environmental related technologies such as fuel cell, chemical reactors for organic synthesis, and environmental remediation. Therefore, this review aims to critically analyze the recent progress on single-atom catalysts (SACs) application in oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and chemical and/or electrochemical organic transformations. Finally, opportunities that may open up in the future are summarized, along with suggesting new applications for possible exploitation of SACs.

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The rational design of single-atom catalysts for electrochemical ammonia synthesis via a descriptor-based approach

Abstract: Single-atom catalysts (SACs) have been studied widely in electrocatalysis towards renewable energy conversion. Herein, we present a general descriptor-based strategy for the rational design of SACs via density functional theory...

Cited by 63 publications

References 48 publications

Toward computational design of chemical reactions with reaction phase diagram

Toward computational design of chemical reactions with reaction phase diagram

Os₁B₁₁N₁₂/C₂N as an Efficient Electrocatalyst for Nitrogen Reduction Reaction

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

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The rational design of single-atom catalysts for electrochemical ammonia synthesis via a descriptor-based approach

Abstract: Single-atom catalysts (SACs) have been studied widely in electrocatalysis towards renewable energy conversion. Herein, we present a general descriptor-based strategy for the rational design of SACs via density functional theory...

Cited by 63 publications

References 48 publications

Toward computational design of chemical reactions with reaction phase diagram

Toward computational design of chemical reactions with reaction phase diagram

Os1B11N12/C2N as an Efficient Electrocatalyst for Nitrogen Reduction Reaction

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

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Os₁B₁₁N₁₂/C₂N as an Efficient Electrocatalyst for Nitrogen Reduction Reaction