Key Takeaways & Executive Findings
- •• • C2+ Faradaic efficiency of 80.4% at 800 mA cm−2: This exceeds typical Cu-based catalysts (often <70% at such high current densities), directly addressing the industrial requirement for high selectivity at ampere-level currents, reducing downstream separation costs. • • Rate-determining hydrogenation barrier reduced by 0.16 eV: DFT calculations show that Cu(100)/Cu(110) interfaces lower the energy barrier for *CO hydrogenation to *CHO, enabling faster kinetics and higher turnover rates, critical for maintaining performance under industrial load. • • Kilogram-scale brochantite nanosheet precursors: The synthesis is scalable, producing gram to kilogram quantities, which is essential for transitioning from laboratory to industrial electrolyzer stacks, mitigating supply chain bottlenecks. • • Operando Raman evidence of sufficient *CO surface coverage: The abundant interfaces sustain high *CO coverage, promoting C–C coupling and suppressing competing hydrogen evolution, as evidenced by the high C2+ selectivity at 800 mA cm−2.
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Abstract
Electroreduction-derived Cu-based two-dimensional materials are promising catalysts for CO2 conversion to C2+ products, yet the role of reconstructed interface structures remains ambiguous. We fabricate interface-engineered Cu nanosheets via in situ pre-electrolysis of kilogram-scale brochantite nanosheet precursors. Lead underpotential deposition and OH− electrosorption analysis confirm abundant Cu(100)/Cu(110) interfaces. In situ attenuated total reflection-surface enhanced infrared absorption spectroscopy reveals C–C coupling pathways involving hydrogenation of *CO to *CHO, followed by coupling to *COCHO. Operando Raman spectra demonstrate that these interfaces provide sufficient *CO surface coverage, facilitating deep coupling reactions. Density-functional-theory calculations indicate that Cu(100)/Cu(110) interfaces reduce the energy barrier of the rate-determining hydrogenation step by 0.16 eV and promote *CO and *CHO coupling. Consequently, the Cu nanosheets achieve a C2+ Faradaic efficiency of 80.4% at an industrial current density of 800 mA cm−2, surpassing most reported Cu-based catalysts. This work establishes a molecular-level understanding of interface engineering for CO2 electroreduction, leveraging scalable precursor synthesis and precise characterization.
1. Introduction
CO2 electroreduction powered by renewable energy offers a route to close the carbon cycle and produce value-added multicarbon (C2+) products, which have high economic value (>$500 t−1) and energy density (>1300 kJ mol−1). Cu-based materials are the leading candidates for converting CO2 to C2+ products, but they suffer from suboptimal reaction rates and low product selectivity, hindering industrial application. The similar thermodynamic potentials of C2+ products, multiple electron/proton transfer steps, and sluggish C–C coupling kinetics collectively result in poor activity and selectivity. Two-dimensional (2D) materials have gained attention due to uniformly exposed facets and abundant coordination-unsaturated sites, but their synthesis is challenging, often requiring high temperatures and pressures and yielding impure morphologies.
Electrochemical in situ topological transformation is a robust strategy for preparing 2D nanosheets, and the electroreduction process can generate surface structures such as grain boundaries. However, limited research has investigated the effects of interface engineering in derived Cu nanosheets for CO2 electroreduction at industrial current densities. This study addresses this gap by designing Cu(100)/Cu(110) interface-confined Cu nanosheets via in situ pre-electrolysis of kilogram-scale brochantite precursors. The interface structures are characterized by lead underpotential deposition and OH− electrosorption, and the reaction pathway is elucidated using in situ ATR-SEIRAS and operando Raman spectroscopy. DFT calculations reveal reduced energy barriers for key steps, and the catalyst achieves a C2+ Faradaic efficiency of 80.4% at 800 mA cm−2, demonstrating a molecular-level understanding of interface engineering for industrial CO2 electroreduction.
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Qiong Wu, Runhua Chen, Juncheng Zhu, Shumin Wang, Yang Wu, Yongfu Sun (2025). In situ reconstructed interface-engineered Cu nanosheets for industrial-current-density CO2 electroreduction to C2+ products. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3392-8
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Frequently Asked Questions
What is the long-term stability of the Cu(100)/Cu(110) interface-engineered nanosheets under industrial current densities, and what degradation mechanisms are observed?
The paper reports a C2+ Faradaic efficiency of 80.4% at 800 mA cm−2, but does not provide long-term stability data. Typical Cu-based catalysts suffer from reconstruction, poisoning, and electrode flooding under prolonged operation. The in situ reconstructed interfaces may be susceptible to further structural evolution, leading to performance decay. Industrial deployment requires stability tests exceeding 1000 hours; thus, accelerated stress tests and post-mortem analyses are necessary to identify failure modes such as Cu dissolution, carbonate deposition, or loss of interface density.
How does the cost of producing kilogram-scale brochantite nanosheet precursors compare with conventional Cu nanoparticle synthesis, and what are the scalability bottlenecks?
The synthesis of brochantite nanosheets is described as kilogram-scale, but no cost analysis is provided. Brochantite (Cu4SO4(OH)6) synthesis typically involves aqueous precipitation from copper salts, which is cost-effective. However, the subsequent in situ pre-electrolysis to form Cu nanosheets adds electrochemical processing steps. Scalability bottlenecks include uniform electrode coating, electrolyte management, and maintaining interface density across large-area electrodes. Techno-economic analysis is needed to assess if the added complexity translates to sufficient performance gains to offset higher capital and operating costs.
What is the Faradaic efficiency for individual C2+ products (e.g., ethylene, ethanol, acetate) and how does the distribution affect downstream separation economics?
The abstract reports a total C2+ Faradaic efficiency of 80.4% but does not specify the distribution among C2+ products. Industrial separation of C2+ mixtures (e.g., ethylene, ethanol, acetate) is energy-intensive and costly. A high total C2+ FE is insufficient if the product slate is broad; selectivity for a single high-value product (e.g., ethylene >60%) is preferable. The paper's focus on C–C coupling pathways suggests ethylene and ethanol as major products, but without detailed product quantification, separation costs remain uncertain.
How does the Cu(100)/Cu(110) interface density correlate with performance, and can it be precisely controlled during synthesis?
Lead underpotential deposition and OH− electrosorption confirm abundant Cu(100)/Cu(110) interfaces, but the paper does not quantify interface density or provide a direct correlation with Faradaic efficiency. Control over interface density is achieved via pre-electrolysis conditions, but the window for optimal interface formation may be narrow. Reproducibility at scale requires precise control of potential, time, and precursor morphology. Without quantitative structure–activity relationships, optimizing interface density for maximum C2+ yield remains empirical.
What are the competing side reactions (e.g., hydrogen evolution) at 800 mA cm−2, and how does the interface engineering suppress them?
At 800 mA cm−2, hydrogen evolution reaction (HER) competes with CO2 reduction. The paper reports 80.4% C2+ FE, implying ~19.6% goes to other products, likely H2 and CO. Operando Raman shows sufficient *CO coverage, which suppresses HER by occupying active sites. The Cu(100)/Cu(110) interfaces promote *CO hydrogenation to *CHO and subsequent coupling, outcompeting proton reduction. However, the exact H2 FE is not stated; minimizing HER is critical for maximizing carbon efficiency and reducing separation costs.
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