Atomically Dispersed Reactive Centers for Electrocatalytic CO<sub>2</sub> Reduction and Water Splitting

Zhang, Huabin; Cheng, Weiren; Luan, Deyan; Lou, Xiong Wen David

doi:10.1002/ange.202014112

Cited by 27 publications

(12 citation statements)

References 130 publications

(239 reference statements)

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“…Ideally, atomic dimer/trimers shall be distributed in the support uniformly, and be stabilized through strong metal‐support interactions (SMSI). [ 48 ] Such SMSI will affect not only the stability but also the activity nature for surface reactions. To this end, it would be essential to examine the distribution of atomic sites on the supports and figure out their local bond coordination environment.…”

Section: Integrating Different Single Atomsmentioning

confidence: 99%

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Zhang

Zhu

et al. 2022

Interdisciplinary Materials

146

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Single‐atom catalysts, featuring some of the most unique activities, selectivity, and high metal utilization, have been extensively studied over the past decade. Given their high activity, selectivity, especially towards small molecules or key intermediate conversions, they can be synergized together with other active species (typically other single atoms, atomic clusters, or nanoparticles) in either tandem or parallel or both, leading to much better performance in complex catalytic processes. Although there have been reports on effectively combining the multiple components into one single catalytic entity, the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner. Herein, in this overview, the key synergistic interactions, binary complementary effects, and the bifunctional functions of single atoms with other active species are defined and discussed in detail. The integration functions of their marriages are investigated with particular emphasis on the homogeneous and heterogeneous combinations, spatial distribution, synthetic strategies, and the thus‐derived outstanding catalytic performance, together with new light shined on the catalytic mechanisms by zooming in several case studies. The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited, on the basis of the in situ/operando evidence. Last, we feature the current challenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

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Section: Integrating Different Single Atomsmentioning

confidence: 99%

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Zhang

Zhu

et al. 2022

Interdisciplinary Materials

146

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“…I n recent years, electrocatalytic carbon dioxide reduction reaction (CO 2 RR) has attracted extensive attention from researchers due to its potential application on the mitigation of the greenhouse gas effect and energy crisis. 1−4 Currently, HCOOH and CO account for the majority of reduction products in electrochemical CO 2 RR; 5 on the other hand, hydrocarbons are rare, especially for C 2 H 4 . As the petrochemical capturing the largest volume among other petrochemicals, C 2 H 4 is mainly obtained industrially by the cracking reaction of naphtha and the distillation of cracking gas.…”

mentioning

confidence: 99%

Highly Selective CO₂ Electroreduction to C₂H₄ Using a Metal–Organic Framework with Dual Active Sites

et al. 2021

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Conversion from CO 2 to C 2 H 4 is important for the development of energy and the environment, but the high energy barrier of hydrogenation of the *CO intermediate and C−C coupling step tend to result in C 1 compounds as the main product and thus restrict the generation of C 2 H 4 . Here, we report a metal−organic framework (denoted as PcCu-Cu-O), composed of 2,3,9,10,16,17,23,24-octahydroxyphthalo-cyaninato)copper(II) (PcCu-(OH) 8 ) ligands and the square-planar CuO 4 nodes, as the electrocatalyst for CO 2 to C 2 H 4 . Compared with the discrete molecular copper-phthalocyanine (Faradaic efficiency (FE) of C 2 H 4 = 25%), PcCu-Cu-O exhibits much higher performance for electrocatalytic reduction of CO 2 to C 2 H 4 with a FE of 50(1)% and a current density of 7.3 mA cm −2 at the potential of −1.2 V vs RHE in 0.1 M KHCO 3 solution, representing the best performance reported to date. In-situ infrared spectroscopy and control experiments suggested that the enhanced electrochemical performance may be ascribed to the synergistic effect between the CuPc unit and the CuO 4 unit, namely the CO on the CO-producing site (CuO 4 site) can efficiently migrate and dimerize with the *CO intermediate adsorbed on the C 2 H 4 -producing site (CuPc), giving a lower C−C dimerization energy barrier.

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“…Moreover, when atomic pairs are formed between different atoms, the interactions between the electronic structures might make it possible for the adsorption and desorption of the reaction intermediate to reach a suitable state. Therefore, dual atomic catalysts may show superior activity, higher selectivity, or stability than corresponding single atomic catalysts (33)(34)(35)(36)(37)(38). Also, the combination of transition metal-based single atom and single atomic RE may have unexpected effects on eCRR.…”

Section: Introductionmentioning

confidence: 99%

Tunable CO/H ₂ ratios of electrochemical reduction of CO ₂ through the Zn-Ln dual atomic catalysts

et al. 2021

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Atomically Dispersed Reactive Centers for Electrocatalytic CO₂ Reduction and Water Splitting

Cited by 27 publications

References 130 publications

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Highly Selective CO₂ Electroreduction to C₂H₄ Using a Metal–Organic Framework with Dual Active Sites

Tunable CO/H ₂ ratios of electrochemical reduction of CO ₂ through the Zn-Ln dual atomic catalysts

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Atomically Dispersed Reactive Centers for Electrocatalytic CO2 Reduction and Water Splitting

Cited by 27 publications

References 130 publications

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Highly Selective CO2 Electroreduction to C2H4 Using a Metal–Organic Framework with Dual Active Sites

Tunable CO/H 2 ratios of electrochemical reduction of CO 2 through the Zn-Ln dual atomic catalysts

Contact Info

Product

Resources

About

Atomically Dispersed Reactive Centers for Electrocatalytic CO₂ Reduction and Water Splitting

Highly Selective CO₂ Electroreduction to C₂H₄ Using a Metal–Organic Framework with Dual Active Sites

Tunable CO/H ₂ ratios of electrochemical reduction of CO ₂ through the Zn-Ln dual atomic catalysts