Development of Electrocatalysts for Efficient Nitrogen Reduction Reaction under Ambient Condition

The development of low-cost and highly efficient materials for the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is an attractive and challenging topic in chemistry. In this study, the electrocatalytic performance of a series of transition metal (TM) atoms supported on MoS2 nanosheets (TM@MoS2) was systematically investigated using density functional theory (DFT) calculations. It was found that Re supported on MoS2 (Re@MoS2) has the best NRR catalytic activity with a limiting potential of -0.43 V, along with high selectivity over the competing hydrogen evolution reaction (HER). Moreover, the ab initio molecular dynamics (AIMD) simulations at 500 K and density of states (DOS) calculations indicated the high thermodynamic stability and excellent electrical conductivity of Re@MoS2. A linear trend between several parameters of single atom catalysts (SACs) and the adsorption Gibbs free energy change of the NH species (ΔG*NH) was observed, indicating the later as a simple descriptor for the facilitated screening of novel SACs. These results pave the way for exploring novel, highly efficient electrocatalysts for the electrochemical NRR under ambient conditions.

A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction.

Single-atom catalysts (SACs) stand out from the atomically dispersed catalysts due to their high specific activity and 100% atomic utilization ratio. However, besides inheriting most of the advantages of SACs, multiple-atom centered site catalysts not only boost higher metal atom loading but also provide more flexible active sites. In this work, by using spin-polarized density functional theory calculations, we systematically investigated the electrochemical nitrogen reduction reaction (eNRR) performance catalyzed by Mox (x = 1-4) supported on graphdiyne (GDY). Our results showed that N2 was favorably adsorbed on the substrates via a well-known "acceptance-donation" mechanism, which can be deeply understood by good multiple linear regressions between the adsorption Gibbs free energy of N2 and lengths or integrated crystal orbital Hamilton populations of Mo-N and N-N bonds. According to the designed screening criteria, Mo3@GDY was found to be most active toward NRR with high selectivity and stability. The predicted onset potential was only -0.32 V. The activity originates from a moderate N adsorption energy, which can balance the thermodynamics of the two potential potential-determining steps, i.e., N2 + H+ + e- = *N2H and *NH2 + H+ + e- = NH3. Moreover, the GDY serves as an electron reservoir during the whole NRR process, where it can provide electrons or accept electrons arbitrarily depending on the need of each elementary step, suggesting that the GDY sheet is a very suitable platform for electrocatalysis applications. The superior electrocatalytic performance of the triple-atom catalyst compared to that of the SACs, double-atom catalyst, and the quadruple-atom cluster catalyst toward NRR offers a huge opportunity for the exploration of a new generation of electrochemical catalysts, where the metal clusters should be highlighted.

Screening a Suitable Mo Form Supported on Graphdiyne for Effectively Electrocatalytic N2 Reduction Reaction: From Atomic Catalyst to Cluster Catalyst

Self-propagating synthesis of Zn-loaded biochar for tetracycline elimination.

Carbon allotropes have contributed to all aspects of people's lives throughout human history. As emerging carbon-based low-dimensional materials, graphyne family members (GYF), represented by graphdiyne, have a wide range potential applications due to their superior physical and chemical properties. In particular, graphdiyne (GDY), as the leader of the graphyne family, has been practically applied to various research fields since it was first successfully synthesized. GYF have a large surface area, both sp and sp2 hybridization, and a certain band gap, which was considered to originate from the overlap of carbon 2pz orbitals and the inhomogeneous π-bonds of carbon atoms in different hybridization forms. These properties mean GYF-based materials still have many potential applications to be developed, especially in energy storage and catalytic utilization. Since most of the GYF have yet to be synthesized and applications of successfully synthesized GYF have not been developed for a long time, theoretical results in various application fields should be shared to experimentalists to attract more intentions. In this Review, we summarized and discussed the synthesis, structural properties, and applications of GYF-based materials from the theoretical insights, hoping to provide different viewpoints and comments.

Graphynes and Graphdiynes for Energy Storage and Catalytic Utilization: Theoretical Insights into Recent Advances.

The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N2 reduction reaction

Two-dimensional SiP3 Monolayer as Promising Anode with Record-high Capacity and Fast Diffusion for Alkali-ion Battery

Controllable Oxygen-doping of Two-dimensional Heterostructure as Diode-type Gas Sensor with High Performance

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The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N2 reduction reaction

Two-dimensional SiP3 Monolayer as Promising Anode with Record-high Capacity and Fast Diffusion for Alkali-ion Battery

Controllable Oxygen-doping of Two-dimensional Heterostructure as Diode-type Gas Sensor with High Performance