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In alkaline and neutral MEA CO 2 electrolyzers, CO 2 rapidly converts to (bi)carbonate, imposing a significant energy penalty arising from separating CO 2 from the anode gas outlets. Here we report a CO 2 electrolyzer uses a bipolar membrane (BPM) to convert (bi)carbonate back to CO 2 , preventing crossover; and that surpasses the single-pass utilization (SPU) limit (25% for multi-carbon products, C 2+ ) suffered by previous neutral-media electrolyzers. We employ a stationary unbuffered catholyte layer between BPM and cathode to promote C 2+ products while ensuring that (bi)carbonate is converted back, in situ, to CO 2 near the cathode. We develop a model that enables the design of the catholyte layer, finding that limiting the diffusion path length of reverted CO 2 to ~10 μm balances the CO 2 diffusion flux with the regeneration rate. We report a single-pass CO 2 utilization of 78%, which lowers the energy associated with downstream separation of CO 2 by 10× compared with past systems. In the carbon dioxide (CO 2 ) to multicarbon electrolysis, the crossover CO 2 to the oxygen-rich anodic gas stream add a further energy-intensive chemical separation step. Here, the authors demonstrate a bipolar membrane-based electrolyzer design that eliminates the crossover CO2.

The electrochemical conversion of CO 2 to methane provides a means to store intermittent renewable electricity in the form of a carbon-neutral hydrocarbon fuel that benefits from an established global distribution network. The stability and selectivity of reported approaches reside below technoeconomic-related requirements. Membrane electrode assembly-based reactors offer a known path to stability; however, highly alkaline conditions on the cathode favour C-C coupling and multi-carbon products. In computational studies herein, we find that copper in a low coordination number favours methane even under highly alkaline conditions. Experimentally, we develop a carbon nanoparticle moderator strategy that confines a copper-complex catalyst when employed in a membrane electrode assembly. In-situ XAS measurements confirm that increased carbon nanoparticle loadings can reduce the metallic copper coordination number. At a copper coordination number of 4.2 we demonstrate a CO 2 -to-methane selectivity of 62%, a methane partial current density of 136 mA cm −2 , and > 110 hours of stable operation. Electrochemical conversion of carbon dioxide to methane can store intermittent renewable electricity in a staple of global energy. Here, the authors develop a moderator strategy to maintain the catalyst in a low coordination state, thereby enabling stable and selective electrochemical methanation.

The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources 1 . However, the highly selective generation of economically desirable products such as ethylene from the carbon dioxide reduction reaction (CO 2 RR) remains a challenge 2 . Tuning the stabilities of intermediates to favour a desired reaction pathway can improve selectivity 3 – 5 , and this has recently been explored for the reaction on copper by controlling morphology 6 , grain boundaries 7 , facets 8 , oxidation state 9 and dopants 10 . Unfortunately, the Faradaic efficiency for ethylene is still low in neutral media (60 per cent at a partial current density of 7 milliamperes per square centimetre in the best catalyst reported so far 9 ), resulting in a low energy efficiency. Here we present a molecular tuning strategy—the functionalization of the surface of electrocatalysts with organic molecules—that stabilizes intermediates for more selective CO 2 RR to ethylene. Using electrochemical, operando/in situ spectroscopic and computational studies, we investigate the influence of a library of molecules, derived by electro-dimerization of arylpyridiniums 11 , adsorbed on copper. We find that the adhered molecules improve the stabilization of an ‘atop-bound’ CO intermediate (that is, an intermediate bound to a single copper atom), thereby favouring further reduction to ethylene. As a result of this strategy, we report the CO 2 RR to ethylene with a Faradaic efficiency of 72 per cent at a partial current density of 230 milliamperes per square centimetre in a liquid-electrolyte flow cell in a neutral medium. We report stable ethylene electrosynthesis for 190 hours in a system based on a membrane-electrode assembly that provides a full-cell energy efficiency of 20 per cent. We anticipate that this may be generalized to enable molecular strategies to complement heterogeneous catalysts by stabilizing intermediates through local molecular tuning. Electrocatalytic reduction of CO 2 over copper can be made highly selective by ‘tuning’ the copper surface with adsorbed organic molecules to stabilize intermediates for carbon-based fuels such as ethylene

A very basic pathway from CO2 to ethyleneEthylene is an important commodity chemical for plastics. It is considered a tractable target for synthesizing renewable resources from carbon dioxide (CO2). The challenge is that the performance of the copper electrocatalysts used for this conversion under the required basic reaction conditions suffers from the competing reaction of CO2 with the base to form bicarbonate. Dinh et al. designed an electrode that tolerates the base by optimizing CO2 diffusion to the catalytic sites (see the Perspective by Ager and Lapkin). This catalyst design delivers 70% efficiency for 150 hours.Science, this issue p. 783; see also p. 707Carbon dioxide (CO2) electroreduction could provide a useful source of ethylene, but low conversion efficiency, low production rates, and low catalyst stability limit current systems. Here we report that a copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE). Hydroxide ions on or near the copper surface lower the CO2 reduction and carbon monoxide (CO)–CO coupling activation energy barriers; as a result, onset of ethylene evolution at −0.165 volts versus an RHE in 10 molar potassium hydroxide occurs almost simultaneously with CO production. Operational stability was enhanced via the introduction of a polymer-based gas diffusion layer that sandwiches the reaction interface between separate hydrophobic and conductive supports, providing constant ethylene selectivity for an initial 150 operating hours.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.An amendment to this paper has been published and can be accessed via a link at the top of the paper.

The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm −2 . Upgrading wasted carbon emissions to high-value, multi-carbon products provides an economic route to reduce carbon dioxide levels, but such conversions have proven challenging. Here, authors explore copper adparticles as highly active surfaces that convert CO to n-propanol with high selectivities.

The renewable-energy-powered electrocatalytic conversion of carbon dioxide and carbon monoxide into carbon-based fuels provides a means for the storage of renewable energy. We sought to convert carbon monoxide—an increasingly available and low-cost feedstock that could benefit from an energy-efficient upgrade in value—into n -propanol, an alcohol that can be directly used as engine fuel. Here we report that a catalyst consisting of highly fragmented copper structures can bring C 1 and C 2 binding sites together, and thereby promote further coupling of these intermediates into n -propanol. Using this strategy, we achieved an n -propanol selectivity of 20% Faradaic efficiency at a low potential of −0.45 V versus the reversible hydrogen electrode (ohmic corrected) with a full-cell energetic efficiency of 10.8%. We achieved a high reaction rate that corresponds to a partial current density of 8.5 mA cm –2 for n -propanol. The upgrade of carbon monoxide to higher alcohols offers a route to renewable fuels. Now, Sinton, Sargent and co-workers report a highly fragmented, copper-based catalyst with engineered interfaces between the (111) and (100) facets that promote the coupling of C 1 and C 2 species, leading to enhanced production of n -propanol.

This content analysis of open-ended survey responses compares and contrasts perceptions on supervision from supervisors with experience providing direct peer support services (PS) and supervisors without experience providing direct peer support services (NPS).A 16-item online survey was distributed via the National Association of Peer Supporters (N.A.P.S.) listserv and through peer networks and peer run organizations. Responses from 837 respondents, across 46 US states, were analyzed. Four open ended questions assessed supervisors’ perceptions on differences supervising peer support workers (PSW) as compared to other staff, important qualities of PSW supervisors, roles when supervising a PSW, and concerns about PSWs in the organization. Among NPS and PS, three major differences in themes emerged: the knowledge required of supervisors, understanding of the role of the PSW, and supervisors’ beliefs regarding PSW competencies. PS have a more nuanced understanding of the peer support worker role and the impact of lived experience in the role.

Understanding integrative approaches to mental health care can improve the responsiveness of the mental health system. Complementary and alternative medicine (CAM) use is on the rise. Research documents that many mental health consumers use CAM. This exploratory study attempts to advance awareness of CAM in mental health by examining mental health consumers’ usage of CAM, their experiences in discussing CAM use with providers, and how CAM use relates to mental health recovery. Results show that 72% of the sample uses such methods, and CAM use is associated with recovery. About 54% of respondents feel CAM combined with medication is more effective than medication alone, and many endorse positive beliefs about CAM. Most consumers shared CAM use with their providers, but when they did not, the main reasons were fear of provider judgment and provider attitudes being a deterrent.