Researchers Uncover Key Insights into CO₂ Reduction Using SnO-Based Electrocatalysts
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Researchers Uncover Key Insights into CO₂ Reduction Using SnO-Based Electrocatalysts

26.02.2025 Tohoku University

A research team has identified critical factors influencing the electrochemical reduction of carbon dioxide (CO2RR) using tin monoxide (SnO)-based electrocatalysts. Their study provides a deeper understanding of how structural changes in SnO affect the production of valuable chemicals such as formic acid (HCOOH) and carbon monoxide (CO), both of which play significant roles in fuel production and industrial applications.

The study was published in the journal ACS Catalysis on February 6, 2025.

While Sn-based materials are widely recognized for their cost-effectiveness and non-toxic nature in CO2RR, existing studies have primarily focused on tin dioxide (SnO2), which predominantly produces HCOOH. Through large-scale data mining of experimental CO₂RR literature, the research team identified a significant trend: SnO-based catalysts demonstrate the ability to generate both HCOOH and CO in comparable amounts. However, despite this potential, the structure-activity relationships of SnO in CO₂RR remain underexplored.

To address this gap, the team employed a constant-potential method alongside surface coverage and reconstruction analyses to simulate CO2RR intermediates under reaction conditions. Their findings reveal that the active surface of SnO undergoes electrochemistry-induced oxygen vacancy formation, a process that directs the distribution of C1 products. Comparative simulations between pristine and reconstructed SnO surfaces further highlight how these structural changes influence electrocatalytic performance.

Hao Li, associate professor at Tohoku University's Advanced Institute for Materials Research (WPI-AIMR) and corresponding author of the paper, has commented on the study's significance:

"This study provides new insights into how SnO-based catalysts can be optimized for CO2 conversion. Understanding how surface modification influences product distribution is an essential step towards designing more efficient and selective electrocatalysts."

The research team intends to build on these results by tailoring Sn-based catalysts at the atomic level, with the goal of achieving precise synthesis of CO2RR products. Future efforts will also integrate machine learning techniques to accelerate the prediction of effective electrocatalysts and optimize reaction conditions.

Key data from this study are available in the Digital Catalysis Platform (DigCat: https://www.digcat.org/), the largest catalysis database developed by the Hao Li Lab.

The article processing charge (APC) was supported by the Tohoku University Support Program.

Title: Electrochemical CO2 Reduction on SnO: Insights into C1 Product Dynamic Distribution and Reaction Mechanisms
Authors: Zhongyuan Guo, Tianyi Wang, Heng Liu, Xue Jia, Di Zhang, Li Wei, Jiang Xu*, and Hao Li*
Journal: ACS Catalysis
DOI: 10.1021/acscatal.4c07987
Angehängte Dokumente
  • Summary of Sn-based catalysts for CO2RR: (a) the category of Sn-based catalysts for CO2RR dominated by Sn oxides-based materials (SnOx), which account for approximately 65% of the total; (b) advantages of SnOx compared to other Sn-based materials including high C1 selectivity, the easily tuned morphology, low cost, and simpler synthesis process; (c) the uncovered structure-activity relationship of SnO2-based materials, i.e., (i) the surface-active configurations, (ii) the Gibbs free energy evolutions toward CO and HCOOH, and (iii) the delivered optimal CO2RR performance in experiments; (d) the pivotal but unresolved questions in SnO-catalyzed CO2RR that warrant further investigation, including the surface coverages, surface-active sites, the effects of applied potentials on CO2RR intermediates, and reaction mechanisms of C1 distribution. All literature data including the optimal potentials, CO2RR performance, and the corresponding references were extracted via a large-scale data mining from the experimental CO2RR literature published during the past decade, which can be found in Table S1 and are also available in the DigCat database: https://www.digcat.org/. ©Hao Li
  • Surface coverage and reconstruction of SnO electrocatalysts during CO2RR: (a, b) One-dimensional (1D) surface Pourbaix diagrams of SnO at USHE = 0 and pH = 0, respectively; (c) 2D surface Pourbaix diagram of SnO; (d) a schematic illustration of SnO electroreduction, highlighting varying levels of oxygen vacancy coverage (0 → 1/2 ML OV* → 1/1 ML OV*); (e) migration barrier of lattice oxygen (OL) within SnO nanosheets, along with the associated structures representing the initial (IS), transition (TS), and final states (FS) during the OL migration process; (f) formation free energy of H2(OL)* and OV* on SnO as a function of URHE; (g) the Gibbs free energy of electroreduction-induced OV* formation on p-SnO under the neutral environment at different potentials; (h) the Gibbs free energy associated with the formation of electroreduction-induced OV* on reconstructed SnO with an OV* concentration of 1/2 ML (r-SnO1-x-1/2OV*) under neutral conditions at various applied potentials; (i) surface reconstruction of SnO nanosheets with the first layer fully reduced named as r-SnO1-x-1/1OV*, simulated by AIMD. ©Hao Li
  • CO2RR on reconstructed SnO (r-SnO1-x-1/1Ov*): (a) CO2RR mechanisms toward HCOOH and CO production; (b) ΔEads of key *COOH and *OCHO intermediates in different configurations; (c) CO2RR intermediates on r-SnO1-x-1/1Ov* including the catalyst slab (*), *OCHO, *COOH, and *CO; (d) total electronic energies of r-SnO1-x-1/1Ov* slab, *COOH, *CO, and *OCHO intermediates as the function of applied potentials (V/SHE); (e) ΔEads comparison of *COOH, *OCHO, and *CO intermediates as the function of applied potentials (V/SHE); and (f-i) the Gibbs free energy change of the CO2 elementary reduction step as the function of applied potentials (V/RHE). ©Hao Li
26.02.2025 Tohoku University
Regions: Asia, Japan
Keywords: Science, Physics, Applied science, Engineering

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