Current Opinion in Green and Sustainable Chemistry, Journal Year: 2019, Volume and Issue: 16, P. 47 - 56
Published: Jan. 22, 2019
Language: Английский
Current Opinion in Green and Sustainable Chemistry, Journal Year: 2019, Volume and Issue: 16, P. 47 - 56
Published: Jan. 22, 2019
Language: Английский
Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(12), P. 7610 - 7672
Published: May 22, 2019
To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors impact CO2R activity selectivity, including surface structure, morphology, composition, choice electrolyte ions pH, cell design. Many these often intertwined, which can complicate discovery design efforts. Here we take broad historical view different aspects their complex interplay in catalysis on Cu, with purpose providing new insights, critical evaluations, guidance field regard research directions best practices. First, describe various experimental probes complementary theoretical methods have been used discern mechanisms by products formed, next present our current understanding reaction networks for Cu. We then analyze two key attempts alter selectivity Cu: nanostructuring formation bimetallic electrodes. Finally, offer some perspectives future outlook CO2R.
Language: Английский
Citations
3733Science, Journal Year: 2019, Volume and Issue: 364(6438)
Published: April 25, 2019
BACKGROUND As the world continues to transition toward carbon emissions–free energy technologies, there remains a need also reduce emissions of chemical production industry. Today many world’s chemicals are produced from fossil fuel–derived feedstocks. Electrochemical conversion dioxide (CO 2 ) into feedstocks offers way turn waste valuable products, closing loop. When coupled renewable sources electricity, these products can be made with net negative footprint, helping sequester CO usable goods. Research and development electrocatalytic materials for reduction has intensified in recent years, advances selectivity, efficiency, reaction rate progressing practical implementation. A variety , such as alcohols, oxygenates, synthesis gas (syngas), olefins—staples global Because at substantial scale, switch renewably powered could result impact. The advancement electrochemical technology convert electrons generated power stable form represents one avenue long-term (e.g., seasonal) storage energy. ADVANCES science progress, priority given pinpoint more accurately targets application, economics barriers market entry. It will important scale electrolyzers increase stability catalysts thousands hours continuous operation. Product separation efficient recycling electrolyte managed. petrochemical industry operates massive complicated supply chain heavy capital costs. Commodity markets difficult penetrate priced on feedstock, which is currently inexpensive shale boom. capture costs flue or direct air product unreacted consider. Assuming that technologies apace, what it take disrupt sector, society gain by doing so? This review presents technoeconomic assessment ethylene, ethanol, monoxide, offering target figures merit application. price electricity far largest cost driver. begin match those traditional processes when prices fall below 4 cents per kWh efficiencies reach least 60%. footprint. comparative analysis electrocatalytic, biocatalytic, shows potential yield greatest emissions, provided steady clean available. Additionally, opportunities exist combine range other thermo- biocatalytic slowly electrify existing further upgrade useful chemicals. Technical challenges operating lifetime, discussed. Supply management entrenched industrial competition considered. OUTLOOK There exists increasingly widespread recognition means production. pricing mechanisms being developed seeing increased governmental support. nascent utilization economy gaining traction, startup companies, prizes, research efforts all pursuing new technologies. Recent through use diffusion electrodes pushing current densities selectivities realm use. Despite this remain technical must overcome commercial ultimately decide whether experiences conversion. Reduction using sourced transform commodity fuels.
Language: Английский
Citations
2257Advanced Materials, Journal Year: 2019, Volume and Issue: 31(31)
Published: May 16, 2019
The electrochemical reduction of CO2 is a promising route to convert intermittent renewable energy storable fuels and valuable chemical feedstocks. To scale this technology for industrial implementation, deepened understanding how the reaction (CO2 RR) proceeds will help converge on optimal operating parameters. Here, techno-economic analysis presented with goal identifying maximally profitable products performance targets that must be met ensure economic viability-metrics include current density, Faradaic efficiency, stability. latest computational RR discussed along can contribute rational design efficient, selective, stable electrocatalysts. Catalyst materials are classified according their selectivity interest potential achieve assessed. recent progress opportunities in system electroreduction described. conclude, remaining technological challenges highlighted, suggesting full-cell efficiency as guiding metric impact.
Language: Английский
Citations
1014Accounts of Chemical Research, Journal Year: 2018, Volume and Issue: 51(4), P. 910 - 918
Published: March 23, 2018
ConspectusElectrocatalytic CO2 conversion at near ambient temperatures and pressures offers a potential means of converting waste greenhouse gases into fuels or commodity chemicals (e.g., CO, formic acid, methanol, ethylene, alkanes, alcohols). This process is particularly compelling when driven by excess renewable electricity because the consequent production solar would lead to closing carbon cycle. However, such technology not currently commercially available. While electrolysis in H-cells widely used for screening electrocatalysts, these experiments generally do effectively report on how electrocatalysts behave flow reactors that are more relevant scalable electrolyzer system. Flow also offer control over reagent delivery, which includes enabling use gaseous feed cathode cell. setup provides platform generating much higher current densities (J) reducing mass transport issues inherent H-cells.In this Account, we examine some systems-level strategies have been applied an effort tailor reactor components improve electrocatalytic reduction. utilized schemes can be categorized two primary architectures: Membrane-based cells microfluidic reactors. Each invoke different dynamic mechanisms delivery sites, both demonstrated achieve high (J > 200 mA cm–2) One strategy common architectures improving J gas phase rather than dissolved liquid electrolyte. physical facet presents number challenges go beyond nature electrocatalyst, scrutinize judicious selection modification certain and/or membrane-based profound effect performance. In cells, example, choice either cation exchange membrane (CEM), anion (AEM), bipolar (BPM) affects kinetics ion pathways range applicable electrolyte conditions. extensive studies performed upon properties porous diffusion layers, materials equally A theme pervasive throughout our analyses associated with precise controlled water management electrolyzers, highlight demonstrate importance maintaining adequate cell hydration sustained electrolysis.
Language: Английский
Citations
895Energy & Environmental Science, Journal Year: 2019, Volume and Issue: 12(5), P. 1442 - 1453
Published: Jan. 1, 2019
The substantial implications of high current densities on the local reaction environment and design catalysts for electrochemical CO2 reduction are addressed. presented perspectives also reflect practices within field offer new opportunities both future catalyst system-focused research efforts.
Language: Английский
Citations
888Nature Energy, Journal Year: 2019, Volume and Issue: 4(6), P. 466 - 474
Published: April 22, 2019
Language: Английский
Citations
632Science Advances, Journal Year: 2020, Volume and Issue: 6(8)
Published: Feb. 21, 2020
Recent progress about electrochemical CO 2 reduction toward C 2+ products is reviewed.
Language: Английский
Citations
610Chem, Journal Year: 2018, Volume and Issue: 4(11), P. 2571 - 2586
Published: Sept. 13, 2018
Language: Английский
Citations
589Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(2), P. 2752 - 2906
Published: Aug. 10, 2021
Photoinduced chemical transformations have received in recent years a tremendous amount of attention, providing plethora opportunities to synthetic organic chemists. However, performing photochemical transformation can be quite challenge because various issues related the delivery photons. These challenges barred widespread adoption steps industry. past decade, several technological innovations led more reproducible, selective, and scalable photoinduced reactions. Herein, we provide comprehensive overview these exciting advances, including flow chemistry, high-throughput experimentation, reactor design scale-up, combination photo- electro-chemistry.
Language: Английский
Citations
540ACS Energy Letters, Journal Year: 2017, Volume and Issue: 3(1), P. 193 - 198
Published: Dec. 18, 2017
Cost competitive electroreduction of CO2 to CO requires electrochemical systems that exhibit partial current density (jCO) exceeding 150 mA cm–2 at cell overpotentials (|ηcell|) less than 1 V. However, achieving such benchmarks remains difficult. Here, we report the on a supported gold catalyst in an alkaline flow electrolyzer with performance levels close economic viability criteria. Onset production occurred and cathode just −0.25 −0.02 V, respectively. High jCO (∼99, 158 cm–2) was obtained low |ηcell| (∼0.70, 0.94 V) high energetic efficiency (∼63.8, 49.4%). The stable for least 8 h. Additionally, onset potentials, kinetic isotope effect, Tafel slopes indicate overpotential media be result pH-independent rate-determining step (i.e., electron transfer) contrast pH-dependent overall process.
Language: Английский
Citations
451