Abstract
Electrochemical carbon dioxide recycling provides an attractive approach to synthesizing fuels and chemical feedstocks using renewable energy. On the path to deploying this technology, basic and applied scientific hurdles remain. Integrating catalytic design with mechanistic understanding yields scientific insights and progresses the technology towards industrial relevance. Catalysts must be able to generate valuable carbon-based products with better selectivity, lower overpotentials and improved current densities with extended operation. Here, we describe progress and identify mechanistic questions and performance metrics for catalysts that can enable carbon-neutral renewable energy storage and utilization.
This is a preview of subscription content, access via your institution
Relevant articles
Open Access articles citing this article.
-
Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products
Nature Communications Open Access 05 October 2023
-
Constructing asymmetric double-atomic sites for synergistic catalysis of electrochemical CO2 reduction
Nature Communications Open Access 03 October 2023
-
Halide-guided active site exposure in bismuth electrocatalysts for selective CO2 conversion into formic acid
Nature Catalysis Open Access 17 August 2023
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Rent or buy this article
Prices vary by article type
from$1.95
to$39.95
Prices may be subject to local taxes which are calculated during checkout







References
Smil, V. Energy Transitions: History, Requirements, Prospects (Praeger, Santa Barbara, 2010).
Chu, S. & Majumdar, A. Opportunities and challenges for a sustainable energy future. Nature 488, 294–303 (2012).
Chu, S., Cui, Y. & Liu, N. The path towards sustainable energy. Nat. Mater. 16, 16–22 (2016).
Obama, B. The irreversible momentum of clean energy. Science 355, 126–129 (2017).
Gao, D., Arán-Ais, R. M., Jeon, H. S. & Roldán Cuenya, B. Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products. Nat. Catal. 2, 198–210 (2019).
Handoko, A. D., Wei, F., Jenndy, Yeo, B. S. & Seh, Z. W. Understanding heterogeneous electrocatalytic carbon dioxide reduction through operando techniques. Nat. Catal. 1, 922–934 (2018). A comprehensive review of state-of-the-art characterization of CO 2 RR electrocatalysts under working conditions.
Kim, D., Sakimoto, K. K., Hong, D. & Yang, P. Artificial photosynthesis for sustainable fuel and chemical production. Angew. Chem. Int. Ed. 54, 3259–3266 (2015).
Hori, Y. in Modern Aspects of Electrochemistry (Springer, 2008). This chapter provides a comprehensive summary of CO 2 RR electrochemistry on a variety of metal surfaces.
Seh, Z. W. et al. Combining theory and experiment in electrocatalysis: insights into materials design. Science 355, eaad4998 (2017). This review describes the interplay between experiment and theory in electrocatalysis for a variety of reactions, as well as introducing intermediate binding strength and scaling relations as frameworks for understanding catalytic activity.
Göttle, A. J. & Koper, M. T. M. Proton-coupled electron transfer in the electrocatalysis of CO2 reduction: prediction of sequential vs. concerted pathways using DFT. Chem. Sci. 8, 458–465 (2017).
Singh, M. R., Clark, E. L. & Bell, A. T. Effects of electrolyte, catalyst, and membrane composition and operating conditions on the performance of solar-driven electrochemical reduction of carbon dioxide. Phys. Chem. Chem. Phys. 17, 18924–18936 (2015).
Weiss, R. F. Carbon dioxide in water and seawater: the solubility of a non-ideal gas. Mar. Chem. 2, 203–215 (1974).
Singh, M. R., Kwon, Y., Lum, Y., Ager, J. W. & Bell, A. T. Hydrolysis of electrolyte cations enhances the electrochemical reduction of CO2 over Ag and Cu. J. Am. Chem. Soc. 138, 13006–13012 (2016).
Wuttig, A., Yaguchi, M., Motobayashi, K., Osawa, M. & Surendranath, Y. Inhibited proton transfer enhances Au-catalyzed CO2-to-fuels selectivity. Proc. Natl Acad. Sci. 113, E4585–E4593 (2016).
Lee, C. W., Cho, N. H., Yang, K. D. & Nam, K. T. Reaction mechanisms of the electrochemical conversion of carbon dioxide to formic acid on tin oxide electrodes. ChemElectroChem 4, 2130–2136 (2017).
Hansen, H. A., Varley, J. B., Peterson, A. A. & Nørskov, J. K. Understanding trends in the electrocatalytic activity of metals and enzymes for CO2 reduction to CO. J. Phys. Chem. Lett. 4, 388–392 (2013).
Feaster, J. T. et al. Understanding selectivity for the electrochemical reduction of carbon dioxide to formic acid and carbon monoxide on metal electrodes. ACS Catal. 7, 4822–4827 (2017).
Baruch, M. F., Pander, J. E., White, J. L. & Bocarsly, A. B. Mechanistic insights into the reduction of CO2 on tin electrodes using in situ ATR-IR spectroscopy. ACS Catal. 5, 3148–3156 (2015).
Kuhl, K. P., Cave, E. R., Abram, D. N. & Jaramillo, T. F. New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces. Energy Environ. Sci. 5, 7050–7059 (2012). Sixteen distinct products are accounted for from CO 2 RR on a polycrystalline Cu surface, providing insight into the competing reaction pathways for multi-carbon product formation on Cu surfaces.
Hori, Y., Takahashi, R., Yoshinami, Y. & Murata, A. Electrochemical reduction of CO at a copper electrode. J. Phys. Chem. B 101, 7075–7081 (1997).
Schmid, B. et al. Reactivity of copper electrodes towards functional groups and small molecules in the context of CO2 electro-reductions. Catalysts 7, 161 (2017).
Kortlever, R., Shen, J., Schouten, K. J. P., Calle-Vallejo, F. & Koper, M. T. M. Catalysts and reaction pathways for the electrochemical reduction of carbon dioxide. J. Phys. Chem. Lett. 6, 4073–4082 (2015).
Goodpaster, J. D., Bell, A. T. & Head-Gordon, M. Identification of possible pathways for C–C bond formation during electrochemical reduction of CO2: new theoretical insights from an improved electrochemical model. J. Phys. Chem. Lett. 7, 1471–1477 (2016).
Liu, X. et al. Understanding trends in electrochemical carbon dioxide reduction rates. Nat. Commun. 8, 15438 (2017).
Hall, A. S., Yoon, Y., Wuttig, A. & Surendranath, Y. Mesostructure-induced selectivity in CO2 reduction catalysis. J. Am. Chem. Soc. 137, 14834–14837 (2015).
Zhang, Y. J., Sethuraman, V., Michalsky, R. & Peterson, A. A. Competition between CO2 reduction and H2 evolution on transition-metal electrocatalysts. ACS Catal. 4, 3742–3748 (2014).
Cave, E. R. et al. Trends in the catalytic activity of hydrogen evolution during CO2 electroreduction on transition metals. ACS Catal. 8, 3035–3040 (2018).
Ross, M. B. et al. Electrocatalytic rate alignment enhances syngas generation. Joule 3, 257–264 (2019).
Liu, M. et al. Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration. Nature 537, 382–386 (2016).
Chen, L. D., Urushihara, M., Chan, K. & Nørskov, J. K. Electric field effects in electrochemical CO2 reduction. ACS Catal. 6, 7133–7139 (2016).
Pérez-Gallent, E., Marcandalli, G., Figueiredo, M. C., Calle-Vallejo, F. & Koper, M. T. M. Structure- and potential-dependent cation effects on CO reduction at copper single-crystal electrodes. J. Am. Chem. Soc. 139, 16412–16419 (2017).
Perez-Gallent, E., Figueiredo, M. C., Calle-Vallejo, F. & Koper, M. T. M. Spectroscopic observation of a hydrogenated CO dimer intermediate during CO reduction on Cu(100) electrodes. Angew. Chem. Int. Ed. 129, 3675–3678 (2017).
Rosen, B. A. et al. Ionic liquid-mediated selective conversion of CO2 to CO at low overpotentials. Science 334, 643–644 (2011).
Urushihara, M., Chan, K., Shi, C. & Nørskov, J. K. Theoretical Study of EMIM+ Adsorption on Silver Electrode Surfaces. J. Phys. Chem. C. 119, 20023–20029 (2015).
Han, Z., Kortlever, R., Chen, H.-Y., Peters, J. C. & Agapie, T. CO2 reduction selective for C2+ products on polycrystalline copper with N-substituted pyridinium additives. ACS Cent. Sci. 3, 853–859 (2017).
Verma, S., Kim, B., Jhong, H. R. M., Ma, S. & Kenis, P. J. A. A gross-margin model for defining technoeconomic benchmarks in the electroreduction of CO2. ChemSusChem 9, 1972–1979 (2016). This work presents a thorough technoeconomic analysis of CO 2 reduction at the device level, explicitly describing how to treat capital costs, catalyst durability and electricity prices.
Jouny, M., Luc, W. W. & Jiao, F. A general techno-economic analysis of CO2 electrolysis systems. Ind. Eng. Chem. Res. 57, 2165–2177 (2018).
Bushuyev, O. S. et al. What should we make with CO2 and how can we make it? Joule 2, 825–832 (2018).
Hoang, T. T. H. et al. Nano porous copper-silver alloys by additive-controlled electro-deposition for the selective electroreduction of CO2 to ethylene and ethanol. J. Am. Chem. Soc. 140, 5791–5797 (2018).
Verma, S. et al. Insights into the low overpotential electroreduction of CO2 to CO on a supported gold catalyst in an alkaline flow electrolyzer. ACS Energy Lett. 3, 193–198 (2018).
Ma, S. et al. One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer. J. Power Sources 301, 219–228 (2016).
Dinh, C. et al. Sustained high-selectivity CO2 electroreduction to ethylene via hydroxide-mediated catalysis at an abrupt reaction interface. Science 360, 783–787 (2018). This work illustrates how the design of an electrolyser system can dramatically improve performance, here, particularly for the synthesis of ethylene.
Jhong, H. R. M., Ma, S. & Kenis, P. J. Electrochemical conversion of CO2 to useful chemicals: current status, remaining challenges, and future opportunities. Curr. Opin. Chem. Eng. 2, 191–199 (2013).
Ripatti, D. S., Veltman, T. R. & Kanan, M. W. Carbon monoxide gas diffusion electrolysis that produces concentrated C2 products with high single-pass conversion. Joule 3, 240–256 (2019).
Yang, H., Kaczur, J. J., Sajjad, S. D. & Masel, R. I. Electrochemical conversion of CO2 to formic acid utilizing SustainionTM membranes. J. CO2 Util. 20, 208–217 (2017).
Burdyny, T. & Smith, W. A. CO2 reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions. Energy Environ. Sci. 12, 1442–1453 (2019).
Chen, Y. & Kanan, M. W. Tin oxide dependence of the CO2 reduction efficiency on tin electrodes and enhanced activity for tin/tin oxide thin-film catalysts. J. Am. Chem. Soc. 134, 1986–1989 (2012). The first demonstration of the oxide-derived approach in CO 2 RR electrocatalysis that has consistently been shown to improve activity and selectivity.
Luc, W. et al. Ag-Sn bimetallic catalyst with a core-shell structure for CO2 reduction. J. Am. Chem. Soc. 139, 1885–1893 (2017).
Kim, D., Resasco, J., Yu, Y., Asiri, A. M. & Yang, P. Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold-copper bimetallic nanoparticles. Nat. Commun. 5, 4948 (2014).
Christophe, J., Doneux, T. & Buess-Herman, C. Electroreduction of carbon dioxide on copper-based electrodes: activity of copper single crystals and copper-gold alloys. Electrocatalysis 3, 139–146 (2012).
Kim, D. et al. Electrochemical activation of CO2 through atomic ordering transformations of AuCu nanoparticles. J. Am. Chem. Soc. 139, 8329–8336 (2017).
Ross, M. B. et al. Tunable Cu enrichment enables designer syngas electrosynthesis from CO2. J. Am. Chem. Soc. 139, 9359–9363 (2017).
Durand, W. J., Peterson, A. A., Studt, F., Abild-Pedersen, F. & Nørskov, J. K. Structure effects on the energetics of the electrochemical reduction of CO2 by copper surfaces. Surf. Sci. 605, 1354–1359 (2011).
Zhu, W. et al. Active and selective conversion of CO2 to CO on ultrathin Au nanowires. J. Am. Chem. Soc. 136, 16132–16135 (2014).
Hong, X., Chan, K., Tsai, C. & Norskov, J. K. How doped MoS2 breaks transition-metal scaling relations for CO2 electrochemical reduction. ACS Catal. 6, 4428–4437 (2016).
Handoko, A. D., Khoo, K. H., Tan, T. L., Jin, H. & Seh, Z. W. Establishing new scaling relations on two-dimensional MXenes for CO2 electroreduction. J. Mater. Chem. A 6, 21885–21890 (2018).
Hori, Y., Wakebe, H., Tsukamoto, T. & Koga, O. Electrocatalytic process of CO selectivity in electrochemical reduction of CO2 at metal electrodes in aqueous media. Electrochim. Acta 39, 1833–1839 (1994).
Hori, Y., Takahashi, I., Koga, O. & Hoshi, N. Selective formation of C2 compounds from electrochemical reduction of CO2 at a series of copper single crystal electrodes. J. Phys. Chem. B 106, 15–17 (2002).
Calle-Vallejo, F. & Koper, M. T. M. Theoretical considerations on the electroreduction of CO to C2 Species on Cu(100) electrodes. Angew. Chem. Int. Ed. 52, 7282–7285 (2013).
Schouten, K. J. P., Qin, Z., Gallent, E. P. & Koper, M. T. M. Two pathways for the formation of ethylene in CO reduction on single-crystal copper electrodes. J. Am. Chem. Soc. 134, 9864–9867 (2012).
Montoya, J. H., Shi, C., Chan, K. & Nørskov, J. K. Theoretical Insights into a CO dimerization mechanism in CO2 electroreduction. J. Phys. Chem. Lett. 6, 2032–2037 (2015).
Sandberg, R. B., Montoya, J. H., Chan, K. & Nørskov, J. K. CO-CO coupling on Cu facets: coverage, strain and field effects. Surf. Sci. 654, 56–62 (2016).
Huang, Y., Handoko, A. D., Hirunsit, P. & Yeo, B. S. Electrochemical reduction of CO2 using copper single-crystal surfaces: effects of CO* coverage on the selective formation of ethylene. ACS Catal. 7, 1749–1756 (2017).
Roberts, F. S., Kuhl, K. P. & Nilsson, A. High selectivity for ethylene from carbon dioxide reduction over copper nanocube electrocatalysts. Angew. Chem. Int. Ed. 54, 5179–5182 (2015).
Gao, D. et al. Plasma-activated copper nanocube catalysts for efficient carbon dioxide electroreduction to hydrocarbons and alcohols. ACS Nano 11, 4825–4831 (2017).
Loiudice, A. et al. Tailoring copper nanocrystals towards C2 products in electrochemical CO2 reduction. Angew. Chem. Int. Ed. 55, 5789–5792 (2016).
Grosse, P. et al. Dynamic changes in the structure, chemical state and catalytic selectivity of Cu nanocubes during CO2 electroreduction: size and support effects. Angew. Chem. Int. Ed. 130, 6300–6305 (2018).
Li, C. W. & Kanan, M. W. CO2 reduction at low overpotential on Cu electrodes resulting from the reduction of thick Cu2O films. J. Am. Chem. Soc. 134, 7231–7234 (2012).
Li, C. W., Ciston, J. & Kanan, M. W. Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper. Nature 508, 504–507 (2014).
Verdaguer-Casadevall, A. et al. Probing the active surface sites for CO reduction on oxide-derived copper electrocatalysts. J. Am. Chem. Soc. 137, 9808–9811 (2015).
Kas, R. et al. Electrochemical CO2 reduction on Cu2O-derived copper nanoparticles: controlling the catalytic selectivity of hydrocarbons. Phys. Chem. Chem. Phys. 16, 12194–12201 (2014).
Ren, D. et al. Selective electrochemical reduction of carbon dioxide to ethylene and ethanol on copper(I) oxide catalysts. ACS Catal. 5, 2814–2821 (2015).
Mistry, H. et al. Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene. Nat. Commun. 7, 12123 (2016).
Kas, R., Kortlever, R., Yilmaz, H., Koper, M. T. M. & Mul, G. Manipulating the hydrocarbon selectivity of copper nanoparticles in CO2 electroreduction by process conditions. ChemElectroChem 2, 354–358 (2015).
Lum, Y., Yue, B., Lobaccaro, P., Bell, A. T. & Ager, J. W. Optimizing C–C coupling on oxide-derived copper catalysts for electrochemical CO2 reduction. J. Phys. Chem. C. 121, 14191–4203 (2017).
Ren, D., Fong, J. & Yeo, B. S. The effects of currents and potentials on the selectivities of copper toward carbon dioxide electroreduction. Nat. Commun. 9, 925 (2018).
Bertheussen, E. et al. Electroreduction of CO on polycrystalline copper at low overpotentials. ACS Energy Lett. 3, 634–640 (2018).
Dutta, A., Rahaman, M., Luedi, N. C., Mohos, M. & Broekmann, P. Morphology matters: tuning the product distribution of CO2 electroreduction on oxide-derived Cu foam catalysts. ACS Catal. 6, 3804–3814 (2016).
Kim, D., Kley, C. S., Li, Y. & Yang, P. Copper nanoparticle ensembles for selective electroreduction of CO2 to C2-C3 products. Proc. Natl Acad. Sci. 114, 10560–10565 (2017). This work demonstrates the importance of Cu structural dynamics in electrolytic conditions that produce multi -carbon products.
Feng, X., Jiang, K., Fan, S. & Kanan, M. W. A direct grain-boundary-activity correlation for CO electroreduction on Cu nanoparticles. ACS Cent. Sci. 2, 169–174 (2016).
Li, Y. et al. Structure-sensitive CO2 electroreduction to hydrocarbons on ultrathin five-fold twinned copper nanowires. Nano Lett. 17, 1312–1317 (2017).
De Luna, P. et al. Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction. Nat. Catal. 1, 103–110 (2018).
Kim, Y. G., Baricuatro, J. H., Javier, A., Gregoire, J. M. & Soriaga, M. P. The evolution of the polycrystalline copper surface, first to Cu(111) and then to Cu(100), at a fixed CO2RR potential: a study by operando EC-STM. Langmuir 30, 15053–15056 (2014).
Gunathunge, C. M. et al. Spectroscopic observation of reversible surface reconstruction of copper electrodes under CO2 reduction. J. Phys. Chem. C. 121, 12337–12344 (2017).
Weng, Z. et al. Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction. Nat. Commun. 9, 415 (2018).
Xiao, H., Cheng, T. & Goddard, W. A. Atomistic mechanisms underlying selectivities in C1 and C2 products from electrochemical reduction of CO on Cu(111). J. Am. Chem. Soc. 139, 130–136 (2017).
Bertheussen, E. et al. Acetaldehyde as an intermediate in the electroreduction of carbon monoxide to ethanol on oxide-derived copper. Angew. Chem. Int. Ed. 55, 1450–1454 (2016).
Lum, Y. & Ager, J. W. Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction. Nat. Catal. 2, 86–93 (2019).
Lum, Y., Cheng, T., Goddard, W. A. & Ager, J. W. Electrochemical CO reduction builds solvent water into oxygenate products. J. Am. Chem. Soc. 140, 9337–9340 (2018).
Jouny, M., Luc, W. & Jiao, F. High-rate electroreduction of carbon monoxide to multi-carbon products. Nat. Catal. 1, 748–755 (2018).
Clark, E. L. et al. Explaining the Incorporation of oxygen derived from solvent water into the oxygenated products of CO reduction over Cu. J. Am. Chem. Soc. 141, 4191–4193 (2019).
Hahn, C. et al. Engineering Cu surfaces for the electrocatalytic conversion of CO2: Controlling selectivity toward oxygenates and hydrocarbons. Proc. Natl Acad. Sci. 114, 5918–5923 (2017).
Ren, D., Ang, B. S. H. & Yeo, B. S. Tuning the selectivity of carbon dioxide electroreduction toward ethanol on oxide-derived CuxZn catalysts. ACS Catal. 6, 8239–8247 (2016).
Clark, E. L., Hahn, C., Jaramillo, T. F. & Bell, A. T. Electrochemical CO2 reduction over compressively strained CuAg surface alloys with enhanced multi-carbon oxygenate selectivity. J. Am. Chem. Soc. 139, 15848–15857 (2017).
Ren, D., Wong, N. T., Handoko, A. D., Huang, Y. & Yeo, B. S. Mechanistic insights into the enhanced activity and stability of agglomerated Cu nanocrystals for the electrochemical reduction of carbon dioxide to n-propanol. J. Phys. Chem. Lett. 7, 20–24 (2016).
Chen, C. S., Wan, J. H. & Yeo, B. S. Electrochemical reduction of carbon dioxide to ethane using nanostructured Cu2O-derived copper catalyst and palladium(II) chloride. J. Phys. Chem. C. 119, 26875–26882 (2015).
Jensen, M. T. et al. Scalable carbon dioxide electroreduction coupled to carbonylation chemistry. Nat. Commun. 8, 489 (2017).
Ostapowicz, T. G., Schmitz, M., Krystof, M., Klankermayer, J. & Leitner, W. Carbon dioxide as a C1 building block for the formation of carboxylic acids by formal catalytic hydrocarboxylation. Angew. Chem. Int. Ed. 52, 12119–12123 (2013).
Klankermayer, J., Wesselbaum, S., Beydoun, K. & Leitner, W. Selective catalytic synthesis using the combination of carbon dioxide and hydrogen: catalytic chess at the interface of energy and chemistry. Angew. Chem. Int. Ed. 55, 7296–7343 (2016).
Haas, T., Krause, R., Weber, R., Demler, M. & Schmid, G. Technical photosynthesis involving CO2 electrolysis and fermentation. Nat. Catal. 1, 32–39 (2018).
Zhao, C. et al. Ionic exchange of metal-organic frameworks to access single nickel sites for efficient electroreduction of CO2. J. Am. Chem. Soc. 139, 8078–081 (2017).
Yang, H. Bin et al. Atomically dispersed Ni(I) as the active site for electrochemical CO2 reduction. Nat. Energy 3, 140–147 (2018).
Wang, X. et al. Regulation of coordination number over single Co sites: triggering the efficient electroreduction of CO2. Angew. Chem. Int. Ed. 57, 1944–1948 (2018).
Jiang, K. et al. Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction. Energy Environ. Sci. 11, 893–903 (2018).
Ju, W. et al. Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2. Nat. Commun. 8, 944 (2017).
Zhang, X. et al. Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structures. Nat. Commun. 8, 14675 (2017).
Jackson, M. N. et al. Strong electronic coupling of molecular sites to graphitic electrodes via pyrazine conjugation. J. Am. Chem. Soc. 140, 1004–1010 (2018).
Deng, Y. et al. On the role of sulfur for the selective electrochemical reduction of CO2 to formate on CuSx catalysts. ACS Appl. Mater. Interfaces 10, 28572–28581 (2018).
Zheng, X. et al. Sulfur-modulated tin sites enable highly selective electrochemical reduction of CO2 to formate. Joule 1, 794–805 (2017).
Jain, A. et al. Commentary: the materials project: a materials genome approach to accelerating materials innovation. APL Mater. 1, 011002 (2013).
Bligaard, T. et al. The Brønsted-evans-polanyi relation and the volcano curve in heterogeneous catalysis. J. Catal. 224, 206–217 (2004).
Aspuru-Guzik, A., Lindh, R. & Reiher, M. The matter simulation (R)evolution. ACS Cent. Sci. 4, 144–152 (2018).
Ulissi, Z. W. et al. Machine-learning methods enable exhaustive searches for active bimetallic facets and reveal active site motifs for CO2 reduction. ACS Catal. 7, 6600–6608 (2017).
Ma, X., Li, Z., Achenie, L. E. K. & Xin, H. Machine-learning-augmented chemisorption model for CO2 electroreduction catalyst screening. J. Phys. Chem. Lett. 6, 3528–3533 (2015).
Tran, K. & Ulissi, Z. W. Active learning across intermetallics to guide discovery of electrocatalysts for CO2 reduction and H2 evolution. Nat. Catal. 1, 696–703 (2018).
Singh, A. K., Montoya, J. H., Gregoire, J. M. & Persson, K. A. Robust and synthesizable photocatalysts for CO2 reduction: a data-driven materials discovery. Nat. Commun. 10, 443 (2019).
Huang, L. et al. Catalyst design by scanning probe block copolymer lithography. Proc. Natl Acad. Sci. 115, 3764–3769 (2018).
Nikolaev, P. et al. Autonomy in materials research: a case study in carbon nanotube growth. npj Comput. Mater. 2, 16031 (2016).
Gromski, P. S., Henson, A. B., Granda, J. M. & Cronin, L. How to explore chemical space using algorithms and automation. Nat. Rev. Chem. 3, 119–128 (2019).
Nie, X., Esopi, M. R., Janik, M. J. & Asthagiri, A. Selectivity of CO2 reduction on copper electrodes: the role of the kinetics of elementary steps. Angew. Chem. Int. Ed. 52, 2459–462 (2013).
Liu, X. et al. pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper. Nat. Commun. 10, 32 (2019).
Cheng, T., Fortunelli, A. & Goddard, W. A. III. Reaction intermediates during operando electrocatalysis identified from full solvent quantum mechanics molecular dynamics. Proc. Natl Acad. Sci. 116, 7718–7722 (2019).
Wheeldon, I. et al. Substrate channeling as an approach to cascade reactions. Nat. Chem. 8, 299–309 (2016).
Ye, R., Hurlburt, T. J.,Sabyrov, K., Alayoglu, S. & Somorjai, G. A. Molecular catalysis science: perspective on unifying the fields of catalysis. Proc. Natl Acad. Sci. 113, 5159–5166 (2016).
Irvine, J. T. S. et al. Evolution of the electrochemical interface in high-temperature fuel cells and electrolysers. Nat. Energy 1, 15014 (2016).
Acknowledgements
This work was supported by the CIFAR Bio-Inspired Solar Energy program; by the Ontario Research Fund—Research Excellence Program; by the Director, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, & Biosciences Division, of the US Department of Energy under Contract No. DE-AC02-05CH11231, FWP No. CH030201; and by the Director, Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, of the US Department of Energy under Contract No. DE-AC02-05CH11231. M.B.R. gratefully acknowledges support from the CIFAR Bio-Inspired Solar Energy Program. PDL wishes to thank the Natural Sciences and Engineering Research Council (NSERC) of Canada for support in the form of the Canadian Graduate Scholarship – Doctoral award. D.K. acknowledges support from Samsung Scholarship.
Author information
Authors and Affiliations
Contributions
All authors contributed to the conception and writing of this manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors claim no competing interests.
Additional information
Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Ross, M.B., De Luna, P., Li, Y. et al. Designing materials for electrochemical carbon dioxide recycling. Nat Catal 2, 648–658 (2019). https://doi.org/10.1038/s41929-019-0306-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41929-019-0306-7
This article is cited by
-
Surface passivation for highly active, selective, stable, and scalable CO2 electroreduction
Nature Communications (2023)
-
Best practices for electrochemical reduction of carbon dioxide
Nature Sustainability (2023)
-
Operando studies reveal active Cu nanograins for CO2 electroreduction
Nature (2023)
-
Halide-guided active site exposure in bismuth electrocatalysts for selective CO2 conversion into formic acid
Nature Catalysis (2023)
-
Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products
Nature Communications (2023)