Cu-Ag Tandem Catalysts for High-Rate CO2 Electrolysis toward Multicarbons

Joule, Год журнала: 2020, Номер 4(8), С. 1688 - 1699

Опубликована: Авг. 1, 2020

Язык: Английский

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Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Advanced Energy Materials, Год журнала: 2019, Номер 10(11)

Опубликована: Дек. 20, 2019

Abstract Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites surrounding coordination environments play a significant role in modulating the electronic structure centers, leading to unusual scaling relationships, new reaction mechanisms, improved performance. This review summarizes recent advancements engineering local environment SACs electrocatalytic performance several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution CO 2 nitrogen reaction. Various strategies including heteroatom‐doping, changing location on support, introducing external ligands, constructing dual comprehensively discussed. The controllable synthetic methods activity enhancement mechanism state‐of‐the‐art also highlighted. Recent achievements modification will provide an understanding structure–activity relationship rational design advanced electrocatalysts.

Язык: Английский

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Catalyst–electrolyte interface chemistry for electrochemical CO₂ reduction

Chemical Society Reviews, Год журнала: 2020, Номер 49(18), С. 6632 - 6665

Опубликована: Янв. 1, 2020

The electrochemical reduction of CO2 stores intermittent renewable energy in valuable raw materials, such as chemicals and transportation fuels, while minimizing carbon emissions promoting carbon-neutral cycles. Recent technoeconomic reports suggested economically feasible target products electroreduction the relative influence key performance parameters faradaic efficiency (FE), current density, overpotential practical industrial-scale applications. Furthermore, fundamental factors, available reaction pathways, shared intermediates, competing hydrogen evolution reaction, scaling relations intermediate binding energies, mass transport limitations, should be considered relation to performance. Intensive research efforts have been devoted designing developing advanced electrocatalysts improving mechanistic understanding. More recently, focus was extended catalyst environment, because interfacial region can delicately modulate catalytic activity provide effective solutions challenges that were not fully addressed material development studies. Herein, we discuss importance catalyst-electrolyte interfaces operational based on kinetic equations. extensively review previous studies controlling organic modulators, electrolyte ions, electrode structures, well three-phase boundary at interface. modulates electrocatalytic properties via electronic modification, stabilization, proton delivery regulation, structure reactant concentration control, regulation. We understanding interface its effect activity.

Язык: Английский

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Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications

Advanced Energy Materials, Год журнала: 2020, Номер 10(38)

Опубликована: Авг. 13, 2020

Abstract Electrocatalysis plays a critical role in clean energy conversion, enabling great improvement for future sustainable technologies. Single atom catalysts (SACs) derived from metal–organic framework (MOF) are emerging extraordinary materials electrochemical catalytic applications. Covering the merits of unique electronic structure, low‐coordination environment, quantum size effect, and metal–support interaction, SACs promise enhanced electrocatalytic activity, stability, selectivity field conversion. In this article, MOF synthesis routes to afford well‐dispersed along with respective mechanism systematically reviewed first, typical examples each strategy carefully discussed. Then characterization techniques understanding isolated spatial distribution, local coordination environment SACs, insights into stable mechanisms provided by density functional theory (DFT) calculations summarized. addition, several important applications MOF‐derived including oxygen reduction reaction, CO 2 nitrogen hydrogen evolution etc., highlighted. To facilitate development high‐performing technical challenges corresponding research directions proposed.

Язык: Английский

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Designing CO₂ reduction electrode materials by morphology and interface engineering

Energy & Environmental Science, Год журнала: 2020, Номер 13(8), С. 2275 - 2309

Опубликована: Янв. 1, 2020

This review discusses how morphology and interface engineering promote electrocatalytic CO₂ reduction, providing general design principles to fabricate advanced electrode catalysts.

Язык: Английский

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Carbon-based metal-free electrocatalysts: from oxygen reduction to multifunctional electrocatalysis

Chemical Society Reviews, Год журнала: 2021, Номер 50(21), С. 11785 - 11843

Опубликована: Янв. 1, 2021

Since the discovery of N-doped carbon nanotubes as first carbon-based metal-free electrocatalyst (C-MFEC) for oxygen reduction reaction (ORR) in 2009, C-MFECs have shown multifunctional electrocatalytic activities many reactions beyond ORR, such evolution (OER), hydrogen (HER), dioxide (CO2RR), nitrogen (NRR), and peroxide production (H2O2PR). Consequently, attracted a great deal interest various applications, including metal-air batteries, water splitting devices, regenerative fuel cells, solar chemical production, purification, to mention few. By altering electronic configuration and/or modulating their spin angular momentum, both heteroatom(s) doping structural defects (e.g., atomic vacancy, edge) been demonstrated create catalytic active sites skeleton graphitic materials. Although certain made be comparable or even better than counterparts based on noble metals, transition metals hybrids, further research development are necessary order translate practical applications. In this article, we present timely comprehensive, but critical, review recent advancements field within past five years so by discussing types catalyzed C-MFECs. An emphasis is given potential applications energy conversion storage. The structure-property relationship mechanistic understanding will also discussed, along with current challenges future perspectives.

Язык: Английский

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Identification of Cu(100)/Cu(111) Interfaces as Superior Active Sites for CO Dimerization During CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2021, Номер 144(1), С. 259 - 269

Опубликована: Дек. 28, 2021

The electrosynthesis of valuable multicarbon chemicals using carbon dioxide (CO2) as a feedstock has substantially progressed recently but still faces considerable challenges. A major difficulty lines in the sluggish kinetics forming carbon-carbon (C-C) bonds, especially neutral media. We report here that oxide-derived copper crystals enclosed by six {100} and eight {111} facets can reduce CO2 to products with high Faradaic efficiency 74.9 ± 1.7% at commercially relevant current density 300 mA cm-2 1 M KHCO3 (pH ∼ 8.4). By combining experimental computational studies, we uncovered Cu(100)/Cu(111) interfaces offer favorable local electronic structure enhances *CO adsorption lowers C-C coupling activation energy barriers, performing superior Cu(100) Cu(111) surfaces, respectively. On this catalyst, no obvious degradation was observed over 50 h continuous operation.

Язык: Английский

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Gas diffusion electrode design for electrochemical carbon dioxide reduction

Chemical Society Reviews, Год журнала: 2020, Номер 49(21), С. 7488 - 7504

Опубликована: Янв. 1, 2020

Anthropogenic carbon dioxide (CO2) emissions contribute to the greenhouse effect and global warming, which can lead undesirable climate change extinction of species. Besides ongoing efforts develop environmentally benign sources energy advance technologies for capture sequestration CO2, transformation emitted CO2 into valuable products is a pragmatic solution curb its accumulation in atmosphere. In this regard, electrochemical reduction (ECR) powered by renewable electricity provides an attractive approach because it not only converts fuels chemicals but also offers long-term storage intermittent energies. ECR, gas diffusion electrode (GDE) most critical component has been subject intensive research last few years. This tutorial review insightful guide developing GDEs with high activity, selectivity, stability, three important performance metrics ECR. First, we introduce fundamentals including chemical physical phenomena at electrodes as well cell configurations. Next, discuss recent advances GDE design, focusing on their structure-performance correlation fabrication techniques each GDEs. Finally, remaining challenges propose promising directions design efficient aims promoting development industrially relevant ECR systems bring technology practical applications.

Язык: Английский

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Recent advances in innovative strategies for the CO₂ electroreduction reaction

Energy & Environmental Science, Год журнала: 2020, Номер 14(2), С. 765 - 780

Опубликована: Дек. 15, 2020

This review underlines innovative design strategies for CO₂RR system, also distinctively presents the current status and new trend.

Язык: Английский

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Electrocatalytic CO₂-to-C₂₊ with Ampere-Level Current on Heteroatom-Engineered Copper via Tuning *CO Intermediate Coverage

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(32), С. 14936 - 14944

Опубликована: Авг. 4, 2022

An ampere-level current density of CO2 electrolysis is critical to realize the industrial production multicarbon (C2+) fuels. However, under such a large density, poor CO intermediate (*CO) coverage on catalyst surface induces competitive hydrogen evolution reaction, which hinders reduction reaction (CO2RR). Herein, we report reliable CO2-to-C2+ by heteroatom engineering Cu catalysts. The Cu-based compounds with (N, P, S, O) are electrochemically reduced heteroatom-derived significant structural reconstruction CO2RR conditions. It found that N-engineered (N-Cu) exhibits best productivity remarkable Faradaic efficiency 73.7% -1100 mA cm-2 and an energy 37.2% -900 cm-2. Particularly, it achieves C2+ partial -909 at -1.15 V versus reversible electrode, outperforms most reported In situ spectroscopy indicates adjusts *CO adsorption alters local H proton consumption in solution. Density functional theory studies confirm high strength N-Cu results from depressed HER promoted both bridge atop sites Cu, greatly reduces barrier for C-C coupling.

Язык: Английский

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