Synergistic Enhancement of Electrocatalytic CO2 Reduction to C2 Oxygenates at Nitrogen-Doped Nanodiamonds/Cu Interface

The interfacing of Cu with nitrogen-doped nanodiamond enables the electrocatalytic production of C2 oxygenates from CO2 with promising stability.

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Effective control over electrochemical reduction CO2 to multicarbon products (C≥2) remains a substantial challenge. Of precedent CO2 electrocatalysts, most of them can only generate C1 product such as CO or HCOOH. Nevertheless, examples capable of producing even low to moderate yields of C≥2 products are very limited. Moreover, these catalysts feature low energetic efficiency, high-cost, and poor electrochemical stability, severely hindering their scalable implementation. To address this issue, we explored synergistic effect originating from the interface of two electroactive components to trigger the production of multi-carbon products.

In this work, we report a novel design principle, where a catalytic interface can be rationally assembled through incorporation of Cu nanoparticles into nitrogen-doped nanodiamond (N-ND) giving rise to N-ND/Cu. According to our thorough investigation, the target CO2 to C2 oxygenates transformation indeed occurs at its interface and is beneficial from the synergy of the two components. 

This strategy possesses following advantages: The electrocatalyst is prepared from abundant materials and hence hold promise to serve as a scalable platform; The inherent compositional and electronic tunability from both catalytic components (nanodiamond and Cu) offers an unrivaled degree of control over the  the catalytic interface, and thereby reaction energetics as well as kinetics; The catalyst gives unprecedented high activity and selectivity with respect to literature precedents; The catalyst shows persistent catalytic performance up to 120 h without noticeable activity decay. 

The results highlight the contributions of the rational nanomaterials assembly for tailoring and maintaining reactivity at materials-materials interfaces enabled by nanotechnology approach. We anticipate the design principle of these interfaced materials-materials platform will be applicable to a wide range of catalytic transformations, especially ones with requirement of renewable energy input and aqueous compatibility.

Figure 1. Summary of this work. a) A schematic illustration of preparation of N-ND/Cu composite materials; b) High-resolution TEM (HRTEM) image of N-ND/Cu; c) Electrochemical performance of N-ND/Cu.

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Hongxia Wang

Postdoctoral researcher, Stanford University

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