Insight on Tafel slopes from a microkinetic analysis of aqueous electrocatalysis for energy conversion

Scientific Reports, Год журнала: 2015, Номер 5(1)

Опубликована: Сен. 8, 2015

Abstract Microkinetic analyses of aqueous electrochemistry involving gaseous H 2 or O , i.e., hydrogen evolution reaction (HER), oxidation (HOR), oxygen reduction (ORR) and (OER), are revisited. The Tafel slopes used to evaluate the rate determining steps generally assume extreme coverage adsorbed species (θ ≈ 0 ≈1), although, in practice, coverage-dependent. We conducted detailed kinetic describing coverage-dependent for aforementioned reactions. Our careful provide a general benchmark experimentally observed that can be assigned specific steps. analysis is powerful tool discussing involved electrocatalysis, but our study also demonstrated overly simplified assumptions led an inaccurate description surface electrocatalysis. Additionally, many studies, have been performed conjunction with Butler-Volmer equation, where its applicability regarding only electron transfer kinetics often overlooked. Based on derived HER/HOR as example, limitation expression electrocatalysis discussed this report.

Язык: Английский

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Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction

Chemical Reviews, Год журнала: 2018, Номер 118(5), С. 2302 - 2312

Опубликована: Фев. 6, 2018

Despite the dedicated search for novel catalysts fuel cell applications, intrinsic oxygen reduction reaction (ORR) activity of materials has not improved significantly over past decade. Here, we review role theory in understanding ORR mechanism and highlight descriptor-based approaches that have been used to identify with increased activity. Specifically, by showing performance commonly studied (e.g., metals, alloys, carbons, etc.) is limited unfavorable scaling relationships (for binding energies intermediates), present a number alternative strategies may lead design discovery more promising ORR.

Язык: Английский

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A review on fundamentals for designing oxygen evolution electrocatalysts

Chemical Society Reviews, Год журнала: 2020, Номер 49(7), С. 2196 - 2214

Опубликована: Янв. 1, 2020

The fundamentals related to the oxygen evolution reaction and catalyst design are summarized discussed.

Язык: Английский

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Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide

The Journal of Physical Chemistry Letters, Год журнала: 2015, Номер 6(20), С. 4073 - 4082

Опубликована: Сен. 24, 2015

The electrochemical reduction of CO2 has gained significant interest recently as it the potential to trigger a sustainable solar-fuel-based economy. In this Perspective, we highlight several heterogeneous and molecular electrocatalysts for discuss reaction pathways through which they form various products. Among those, copper is unique catalyst yields hydrocarbon products, mostly methane, ethylene, ethanol, with acceptable efficiencies. As result, substantial effort been invested determine special catalytic properties elucidate mechanism hydrocarbons are formed. These mechanistic insights, together insights on other metals complexes, can provide crucial guidelines design future materials able efficiently selectively reduce useful

Язык: Английский

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Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution

Nature Chemistry, Год журнала: 2017, Номер 9(5), С. 457 - 465

Опубликована: Янв. 9, 2017

Язык: Английский

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Challenges in reduction of dinitrogen by proton and electron transfer

Chemical Society Reviews, Год журнала: 2014, Номер 43(15), С. 5183 - 5191

Опубликована: Янв. 1, 2014

Catalytic reduction of dinitrogen with protons and electrons is a very challenging alternative to the energy expensive Haber–Bosch reaction.

Язык: Английский

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A Review of Electrocatalytic Reduction of Dinitrogen to Ammonia under Ambient Conditions

Advanced Energy Materials, Год журнала: 2018, Номер 8(22)

Опубликована: Май 21, 2018

Abstract The production of ammonia (NH 3 ) from molecular dinitrogen (N 2 under mild conditions is one the most attractive topics in field chemistry. Electrochemical reduction N promising for achieving clean and sustainable NH with lower energy consumption using renewable sources. To date, emerging electrocatalysts electrochemical to at room temperature atmospheric pressure remain largely underexplored. major challenge achieve both high catalytic activity selectivity. Here, recent progress on nitrogen reaction (NRR) ambient theoretical experimental aspects summarized, aiming extracting instructive perceptions future NRR research activities. prevailing theories mechanisms as well computational screening materials are presented. State‐of‐the‐art heterogeneous rational design whole systems involved. Importantly, strategies enhance activity, selectivity, efficiency, stability toward proposed. Moreover, determination methods compared problems relating possible contamination system mentioned so shed fresh light standard protocols measurements.

Язык: Английский

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Electrocatalytic Oxygen Evolution Reaction in Acidic Environments – Reaction Mechanisms and Catalysts

Advanced Energy Materials, Год журнала: 2016, Номер 7(1)

Опубликована: Окт. 26, 2016

The low efficiency of the electrocatalytic oxidation water to O 2 (oxygen evolution reaction‐OER) is considered as one major roadblocks for storage electricity from renewable sources in form molecular fuels like H or hydrocarbons. Especially acidic environments, compatible with powerful proton exchange membrane (PEM), an earth‐abundant OER catalyst that combines high activity and stability still unknown. Current PEM‐compatible catalysts rely mostly on Ir and/or Ru active components, which are both very scarce elements platinum group. Hence, amount has be strictly minimized. Unfortunately, mechanism, most tool optimization, remains unclear. In this review, we first summarize current state our understanding mechanism heterogeneous electrocatalysts, before compare contrast homogenous catalysts. Thereafter, overview over monometallic provided obtain insights into structure‐function relations followed by a review material optimization concepts support materials. Moreover, missing links required complete mechanistic picture well promising pointed out.

Язык: Английский

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Recent Advances and Challenges of Electrocatalytic N₂Reduction to Ammonia

Chemical Reviews, Год журнала: 2020, Номер 120(12), С. 5437 - 5516

Опубликована: Май 27, 2020

Global ammonia production reached 175 million metric tons in 2016, 90% of which is produced from high purity N2 and H2 gases at temperatures pressures via the Haber–Bosch process. Reliance on natural gas for results large energy consumption CO2 emissions. Concerns human-induced climate change are spurring an international scientific effort to explore new approaches reduce its carbon footprint. Electrocatalytic reduction attractive alternative that can potentially enable synthesis under milder conditions small-scale, distributed, on-site electrolysis cells powered by renewable electricity generated solar or wind sources. This review provides a comprehensive account theoretical experimental studies electrochemical nitrogen fixation with focus low selectivity versus protons H2. A detailed introduction detection methods execution control experiments given as they crucial accurate reporting findings. The main part this focuses progress has been achieved range conditions. Finally, comments current challenges potential opportunities field provided.

Язык: Английский

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Toward the Decentralized Electrochemical Production of H₂O₂: A Focus on the Catalysis

ACS Catalysis, Год журнала: 2018, Номер 8(5), С. 4064 - 4081

Опубликована: Март 28, 2018

H2O2 is a valuable, environmentally friendly oxidizing agent with wide range of uses from the provision clean water to synthesis valuable chemicals. The on-site electrolytic production would bring chemical applications beyond its present reach. successful commercialization electrochemical requires cathode catalysts high activity, selectivity, and stability. In this Perspective, we highlight our current understanding factors that control performance. We review influence catalyst material, electrolyte, structure interface at mesoscopic scale. provide original theoretical data on role geometry active site activity selectivity. have also conducted series experiments (i) effect pH glassy carbon, pure metals, metal–mercury alloys, (ii) cell mass transport in liquid half-cells comparison membrane electrode assemblies.

Язык: Английский

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