2026-10-14T03:53:03Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34036691 2026-09-30T19:13:25Z category_1 category_14 category_21 category_873 category_734 category_135 portal_63 item_type_6 month_year_09_2026

Multiscale Regulation of Interfacial Microenvironments for High-Efficiency Electrochemical CO₂ Reduction to C₂₊ Products: A Review and Perspective Weijun Kong (543921) Han Wang (254423) Junhao Tian (25145900) Yuexin Wang (4590040) Yihang Song (13252416) Yanqiang Kong (25145903) Lijun Yang (356935) Biophysics Molecular Biology Biotechnology Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Computational Biology term goal contingent sustainable carbon cycle single optimization strategy several material classes informed neural networks industrial current densities following main conclusions dominant failure modes accepted validation protocols standardized operando datasets molecular reaction network electrocatalysis literature around dimension × four review systematically reorganizes perspective electrochemical reduction 2 </ sub 2 +</ sub achieve higher selectivity respective specific c efficiency electrochemical co ii ), microenvironment reaction pathways operando spectroscopy electrocatalysis rather four scales four dimensions explicit four ), confinement substantial catalyst scale matrix salt precipitation review draws reusable scaffold representative experimental promising route promising direction practical application peak performance next generation multiscale regulation mesoscopic transport mesoscale confinement Electrochemical reduction of CO₂ to high-value C₂₊ products represents a promising route for achieving a sustainable carbon cycle, yet its practical application is hindered by intrinsic challenges in catalyst design, reaction pathways, and carbonate precipitation, which affect the efficiency, selectivity, safety, and lifespan of electrolyzers. This review systematically reorganizes the CO₂-to-C₂₊ electrocatalysis literature around an explicit four-dimension × four-scale matrix (4D × 4S), where the four dimensions are materials engineering (I), confinement/tandem (II), microenvironment/interface regulation (III), and reactor/operation (IV), and the four scales are electronic structure, atomic-to-molecular reaction network, mesoscopic transport, and device-reactor performance. This review draws on representative experimental and computational studies in CO₂-to-C₂⁺ electrocatalysis rather than attempting an exhaustive catalog. We have the following main conclusions: (i) atomic-site design shall cooptimize with mesoscale confinement and microenvironment to achieve higher selectivity at industrial current densities; (ii) membrane-electrode-assembly lifetime, not peak performance, is the central bottleneck for C₂₊ commercialization, with salt precipitation and cation crossover as the dominant failure modes²; (iii) several material classes (atomically defined paired sites, conductive MOFs/COFs, etc.) can maintain high Faraday efficiency of their respective specific C₂₊ products at industrial current densities, but each faces a characteristic trade-off (e.g., lifetime vs. selectivity) that no single optimization strategy can resolve; (iv) Cross-scale theoretical–experimental closure, enabled by operando spectroscopy, machine-learning surrogates, and physics-informed neural networks, is the most promising direction for accelerating the field. The 4D × 4S matrix provides a reusable scaffold for designing and evaluating the next generation of C₂₊ electrocatalysts and electrolyzers, with standardized operando datasets and community-accepted validation protocols as the immediate priorities. We expect that CO₂-to-CO will be the realistic first commercial target, with C₂₊ products as a longer-term goal contingent on substantial catalyst and membrane innovation. 2026-09-30T00:00:00Z Text Journal contribution 10.1021/acs.energyfuels.6c03204.s001 https://figshare.com/articles/journal_contribution/Multiscale_Regulation_of_Interfacial_Microenvironments_for_High-Efficiency_Electrochemical_CO_sub_2_sub_Reduction_to_C_sub_2_sub_Products_A_Review_and_Perspective/34036691 CC BY-NC 4.0