Density Functional Theory for Electrocatalysis

Tuning the electronic structure of a single-atom catalyst (SAC) by controlling its coordination has been recently shown to be a rather promising strategy for further improving its catalytic performance in some electrochemical reactions. Herein, by means of density functional theory (DFT) computations, the impacts of the coordination structure of an Fe–N–C catalyst on its catalytic activity toward the nitrogen reduction reaction (NRR) were explored. Our results revealed that the NRR activity on the central Fe atom can be greatly improved by its coordination with a boron (B) dopant. In particular, the computed limiting potential of the NRR on Fe–B2N2 is −0.65 V, which is the lowest among all B doped Fe–N–C catalysts, suggesting its high NRR catalytic activity. Interestingly, the introduction of B coordination can effectively modulate the interaction of the single Fe atom with the N2H* species, thus improving its NRR catalytic performance. In addition, Fe–B2N2 exhibits high NRR selectivity by effectively suppressing the competing hydrogen evolution reaction (HER) both thermodynamically and kinetically. Therefore, the single Fe catalyst with N and B dual coordination can be utilized as a promising NRR electrocatalyst, which not only highlights the significant effect of local coordination on catalytic activity and selectivity for the NRR, but also provides a new opportunity to further develop more advanced single-atom catalysts for ammonia synthesis.

Coordination tunes the activity and selectivity of the nitrogen reduction reaction on single-atom iron catalysts: a computational study

Single‐atom catalysts, featuring some of the most unique activities, selectivity, and high metal utilization, have been extensively studied over the past decade. Given their high activity, selectivity, especially towards small molecules or key intermediate conversions, they can be synergized together with other active species (typically other single atoms, atomic clusters, or nanoparticles) in either tandem or parallel or both, leading to much better performance in complex catalytic processes. Although there have been reports on effectively combining the multiple components into one single catalytic entity, the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner. Herein, in this overview, the key synergistic interactions, binary complementary effects, and the bifunctional functions of single atoms with other active species are defined and discussed in detail. The integration functions of their marriages are investigated with particular emphasis on the homogeneous and heterogeneous combinations, spatial distribution, synthetic strategies, and the thus‐derived outstanding catalytic performance, together with new light shined on the catalytic mechanisms by zooming in several case studies. The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited, on the basis of the in situ/operando evidence. Last, we feature the current challenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/idm2.12011

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Multi-atom cluster catalysts have turned out to be novel heterogeneous catalysts with atomic dispersion for electrochemical energy applications. Beyond a simple combination of single-atom catalysts, they could offer boosted activity as a result of the synergistic effects between adjacent atoms. Meanwhile, the multiple active sites in the catalytic center may render them versatile binding modes toward adsorbates and provide an opportunity for catalyzing complex reactions with diverse products. Herein, a comprehensive review of the recent development of multi-atom cluster catalysts for electrochemical energy applications is provided. Specifically, the origin of synergistic effects in multi-atom cluster catalysts and related modulation methods are illustrated and summarized. The introduction of multi-atom cluster catalysts to circumvent the scaling relationships as well as their potential for developing new descriptors is then discussed. Subsequently, the methods for fabricating multi-atom cluster catalysts and related characterization techniques are reviewed. This is followed by the discussion of their application in key electrochemical reactions such as water splitting, oxygen reduction, and carbon dioxide/monoxide reduction, as well as the real-time techniques for their mechanistic study. Finally, the future challenges and opportunities concerning the improvement of multi-atom cluster catalysts are outlined, which are essential to make such electrocatalysts viable for electrochemical energy conversion.

/pdf/multi-atom-cluster-catalysts-for-efficient-electrocatalysis-3uc3i6c0.pdf

Multi-atom cluster catalysts for efficient electrocatalysis.

Dispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition

Achieving an effective nitrogen reduction reaction (NRR) under mild conditions is a great challenge for industrial ammonia synthesis. NRR is often accompanied by a competing hydrogen evolution reaction (HER), which causes an extremely low Faraday efficiency. We systematically investigated the NRR reactivity of atom-pair catalysts (APCs) formed by 20 transition metal (TM) elements supported by N-doped graphene via three reaction pathways. By analyzing the correlation among the limiting potential, Gibbs free energy, and d-band center, we evaluated the activity trends of the TM APCs. Our computations revealed that the enzymatic pathway is the most suitable reaction pathway for the TM APCs, and the intrinsic activity trend of these APCs can be determined by the d-band center-based descriptor, which has a simple linear correlation with the bonding/antibonding orbital population. In addition, the NRR APCs with excellent performance have been screened out through selective analysis of the competing HER in the electrocatalytic NRR process.

Atom-Pair Catalysts Supported by N-Doped Graphene for the Nitrogen Reduction Reaction: d-Band Center-Based Descriptor.

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Atom-Pair Catalysts Supported by N-Doped Graphene for the Nitrogen Reduction Reaction: d-Band Center-Based Descriptor.