Key Takeaways & Executive Findings
- •• • Surface Pb-rich Pd3Pb/Pb nanocubes achieve a Faradaic efficiency of 96.88% for C1+ products at −0.72 V vs. RHE, outperforming Pd3Pb/Pd (39.86%) and standard Pd3Pb (81.75%), demonstrating a 2.4-fold improvement over Pd-rich surfaces. • • The 20 nm intermetallic nanocubes with tunable Pb exposure enable isolation of ligand effects from geometric factors, providing a model system for structure-activity correlation studies. • • DFT calculations reveal that Pb incorporation upshifts the d-band center of Pd via p-d hybridization, strengthening intermediate adsorption and lowering energy barriers for C1+ pathways while suppressing HER. • • The synthetic method (one-step solvothermal) yields well-defined nanocubes with controlled surface Pb content, offering a scalable route for precise surface engineering of intermetallic electrocatalysts.
Abstract
A series of ~20 nm intermetallic Pd3Pb nanocubes with tunable surface Pb exposure were synthesized via a facile one-step solvothermal approach, providing an ideal system to investigate the way in which the surface configurations of Pb-rich (Pd3Pb/Pb), Pd-rich (Pd3Pb/Pd), and standard Pd3Pb nanocubes influence the CO2 reduction reaction (CO2RR) mainly through the ligand effect while excluding geometric influences. Electrochemical measurement results indicate that the Pd3Pb/Pb catalyst delivered outstanding C1+ selectivity, achieving a high Faradaic efficiency of 96.88% at −0.72 V (vs. RHE), significantly outperforming the Pd3Pb/Pd (39.86%) and standard Pd3Pb (81.75%) counterparts. In situ FTIR together with DFT calculations further elucidated that Pb incorporation can modulate the electronic structure of Pd via p-d hybridization, leading to the upshift of the d-band center. This will, in return, strengthen the intermediate adsorption ability and lower the energy barriers of the C1+ pathways while effectively suppressing the competing hydrogen evolution reaction. This work establishes a precise surface engineering paradigm of intermetallic nanocrystals for designing high-performance electrocatalysts.
1. Introduction
The electrochemical reduction of CO2 (CO2RR) offers a route to convert waste emissions into valuable chemicals, yet its commercial viability is hampered by the thermodynamic stability of CO2 and the competing hydrogen evolution reaction (HER), which typically results in low Faradaic efficiencies and poor product selectivity. Conventional Pd-based catalysts, while active for CO2RR, suffer from insufficient selectivity and stability under operating conditions. Alloying Pd with p-block elements such as Pb has been explored to modulate electronic structure, but disordered alloys often undergo elemental dissolution, degrading performance over time.
This work addresses these bottlenecks by employing ordered intermetallic Pd3Pb nanocubes with precisely controlled surface Pb exposure. Unlike disordered alloys, intermetallic compounds offer enhanced thermodynamic stability and well-defined atomic arrangements, enabling systematic investigation of surface composition effects. By synthesizing ~20 nm nanocubes with Pb-rich, Pd-rich, and standard surfaces, the authors isolate the ligand effect from geometric influences, demonstrating that Pb-rich surfaces dramatically enhance C1+ selectivity (96.88% FE) while suppressing HER. This surface engineering paradigm provides a robust strategy for designing high-performance, durable CO2RR electrocatalysts.
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LI Junjie, JI Liang, LI Lei, LI Xiao, WU Xingqiao, ZHANG Hui, YANG Deren (2026). Precise Modulation of Surface Pb-Rich Intermetallic Pd3Pb Nanocubes for Efficient Electrocatalytic CO2 Reduction. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4070-2
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Frequently Asked Questions
What is the specific Faradaic efficiency for C1+ products on the Pb-rich Pd3Pb/Pb catalyst, and how does it compare to the Pd-rich and standard counterparts?
The Pb-rich Pd3Pb/Pb catalyst achieves a Faradaic efficiency of 96.88% at −0.72 V vs. RHE, significantly higher than the Pd-rich Pd3Pb/Pd (39.86%) and standard Pd3Pb (81.75%). This indicates that surface Pb enrichment is critical for enhancing C1+ selectivity.
How does the introduction of Pb into the Pd3Pb lattice affect the electronic structure and catalytic activity?
DFT calculations show that Pb hybridizes with Pd via p-d hybridization, upshifting the d-band center. This strengthens intermediate adsorption and lowers energy barriers for C1+ pathways, while suppressing the competing HER, leading to enhanced selectivity and activity.
What is the particle size and morphology of the synthesized catalysts, and how does this influence the CO2RR performance?
The catalysts are ~20 nm nanocubes with well-defined facets. The uniform size and shape allow the study to exclude geometric effects, isolating the ligand effect of surface Pb. This ensures that observed performance differences are solely due to surface composition.
What is the synthetic method used to prepare the Pd3Pb nanocubes, and is it scalable for industrial applications?
The nanocubes are synthesized via a facile one-step solvothermal approach, which is relatively simple and potentially scalable. The method allows precise control over surface Pb exposure, making it suitable for producing high-performance catalysts for practical CO2RR applications.
How does the Pb-rich Pd3Pb/Pb catalyst suppress the hydrogen evolution reaction (HER) compared to other catalysts?
The Pb-rich surface enhances CO2RR selectivity by suppressing HER. The Faradaic efficiency for C1+ products is 96.88%, indicating minimal HER competition. DFT calculations suggest that Pb modification raises the energy barrier for HER, favoring CO2 reduction.
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