Tandem electrocatalytic CO<sub>2</sub> reduction with Fe-porphyrins and Cu nanocubes enhances ethylene production

Wang, Min; Nikolaou, Vasilis; Loiudice, Anna; Sharp, Ian D.; Llobet, Antoni; Buonsanti, Raffaella

doi:10.1039/d2sc04794b

Cited by 25 publications

(28 citation statements)

References 47 publications

(90 reference statements)

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“…A vast library of ligand exchange protocols has been developed and tailored for a multitude of applications. For example, NC-based photovoltaics benefit from the introduction of ligands with short alkyl chains or halide ligands on the NC surface, because these ligands optimize the NC packing density and favor efficient charge transport. , Further, synergistic enhancement of heterogeneous catalysts has been attained by grafting organic species or organometallic complexes to the NC surface. − Finally, NCs functionalized with polyaromatic hydrocarbon (PAH) ligands have emerged as excellent triplet exciton based sensitizers with applications in photocatalysis, ,− optoelelctronics, , optogenetics, , and bioimaging. − …”

Section: Introductionmentioning

confidence: 99%

“…We selected these NCs, as they have historically benefited from being coupled to photoactive ligands. For instance, PbS, CuInS 2 , and CsPbBr 3 passivated by PAH ligands have found great use in incoherent photon conversion and photocatalyst. ,,,− The coupling of PAH ligands with lanthanide-based upconverting nanoparticles (UCNPs) can drastically increase the absorption cross-section of the chromophore/NC hybrids, resulting in a significant enhancement of the upconverted emission intensity. ,, Finally, plasmonic NCs can also be coupled to chromophores, which benefits photo and electrocatalytic applications. − …”

Section: Introductionmentioning

confidence: 99%

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Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

et al. 2023

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Colloidal nanocrystals (NCs) are ideal materials for a variety of applications and devices, which span from catalysis and optoelectronics to biological imaging. Organic chromophores are often combined with NCs as photoactive ligands to expand the functionality of NCs or to achieve optimal device performance. The most common methodology to introduce these chromophores involves ligand exchange procedures. Despite their ubiquitous nature, ligand exchanges suffer from a few limitations, which include reversible binding, restricted access to binding sites, and the need for purification of the samples, which can result in loss of colloidal stability. Herein, we propose a methodology to bypass these inherent issues of ligand exchange through the growth of an amorphous alumina shell by colloidal atomic layer deposition (c-ALD). We demonstrate that c-ALD creates colloidally stable composite materials, which comprise NCs and organic chromophores as photoactive ligands, by trapping the chromophores around the NC core. As representative examples, we functionalize semiconductor NCs, which include PbS, CsPbBr 3 , CuInS 2 , Cu 2−x X, and lanthanide-based upconverting NCs, with polyaromatic hydrocarbons (PAH) ligands. Finally, we prove that triplet energy transfer occurs through the shell and we realize the assembly of a triplet exciton funnel structure, which cannot be obtained via conventional ligand exchange procedures. The formation of these organic/inorganic hybrid shells promises to synergistically boost catalytic and multiexcitonic processes while endowing enhanced stability to the NC core.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

et al. 2023

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“…Most studies on the design of tandem systems have so far focused on the coupling of Cu with a second metallic domain (Zn, 21,22 Au 23 or Ag [24][25][26][27] ) as the CO-generating catalyst. Molecular catalysts, such as cobalt phthalocyanine 28 and iron porphyrin 29,30 have also been successfully employed as the COgenerating catalyst in the context of tandem schemes. Compared to metals, molecular catalysts offer additional versatility for varying the local CO concentration and production rate thanks to the superior chemical tunability via synthetic modications of molecules versus materials.…”

Section: Introductionmentioning

confidence: 99%

“…Compared to metals, molecular catalysts offer additional versatility for varying the local CO concentration and production rate thanks to the superior chemical tunability via synthetic modifications of molecules versus materials. 30 Despite their promise, no experimental work has investigated yet the influence of the spatial arrangement of the components on the catalytic performance of molecular-Cu based tandem systems.…”

Section: Introductionmentioning

confidence: 99%

The spatial distribution of cobalt phthalocyanine and copper nanocubes controls the selectivity towards C₂ products in tandem electrocatalytic CO₂ reduction

et al. 2023

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“…Previous experimental works also propose the tandem electrocatalyst for CO 2 RR on nanocatalysts, where the CO* forms on one type of active site and migrates to other active sites for CC coupling with lower energy barriers. [28,29] Wang et al have reported using the Ni-N-C SACs and Cu nanoparticles as the active sites for the generation of CO* and C 2 products, respectively. [30] The proposed Cu/Ni-N-C has shown high efficiency of 80% FE and a production rate of over 500 mA cm −2 for C 2 products.…”

Section: Introductionmentioning

confidence: 99%

Double‐Dependence Correlations in Graphdiyne‐Supported Atomic Catalysts to Promote CO₂RR toward the Generation of C₂Products

Sun

Wong

et al. 2022

Advanced Energy Materials

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fossil fuels, which account for 70% of the greenhouse gases in the atmosphere and have a profound impact on the global warming issue. Carbon neutrality is critical to address the climate crisis, which requires immediate actions from the global community. China has also set the development goal of reaching the carbon emission peak in 2030 and carbon neutrality in 2060. In recent years, there has been increasing attention and efforts in the technology advances for zero or even negative emissions to accelerate the developments toward carbon neutrality. In particular, carbon capture, utilization, and storage (CCUS) technology are one of the important methods to effectively reduce carbon emissions. As a potential carbon resource compound, carbon dioxide (CO 2 ) can be converted into high-value-added chemicals, carbon-based fuels, and other small molecules with broad applications in industries, which supplies practical solutions for the greenhouse effect. Especially, electrochemical CO 2 reduction reaction (CO 2 RR) represents one of the most promising approaches to capturing and utilizing CO 2 from the atmosphere. [1][2][3] Depending on the electrocatalysts, CO 2 RR can be accomplished via different pathways that involve varied electrons and products from the C 1 products (e.g., CO, HCOOH, and CH 4 ) to valuable C 2 products (e.g., C 2 H 4 , CH 3 CH 2 OH, CH 3 CHO, CH 3 COOH, etc.) for broad applications. [4][5][6][7] Compared to widely reported C 1 products, the generation of complicated C 2 products is still highly challenging with several key bottlenecks to be overcome including large overpotential and low selectivity and faradaic efficiency (FE) of target products, which are attributed to the complicated reaction mechanism with multi-electron transfer processes. [8] Currently, many different electrocatalysts have been reported for CO 2 RR including noble metals and alloys (e.g., Pd, Ag, Au, and Cu), oxides (e.g., Cu x O, SnO 2 , etc.), as well as composite electrocatalysts. [3,[9][10][11][12] However, the generation of valuable multi-carbon products (C 2 and C 2+ products) still mostly depends on the Cu-based electrocatalysts. [3,[13][14][15][16] Recently, the fast developments of atomic catalysts (ACs) have been widely reported in many different energy and Developing efficient and stable atomic catalysts (ACs) to achieve high faradaic efficiency and selectivity of C 2 products is a significant challenge for research on the CO 2 reduction reaction (CO 2 RR). Although significant efforts have been devoted to this endeavor, the understanding of C 2 pathways and the influences of metal selection and active sites on the CO 2 RR still remain unclear. Herein, this work presents a comprehensive theoretical exploration of full C 2 reaction pathway mapping based on graphdiyne (GDY)-supported ACs with considerations of different metals and active sites for the first time. This work demonstrates the integrated large-small cycle mechanism to explain the challenges for C 2 product generation, where the double-dependence correl...

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Tandem electrocatalytic CO₂ reduction with Fe-porphyrins and Cu nanocubes enhances ethylene production

Abstract: Copper-based tandem schemes have emerged as promising strategies to promote the formation of multi-carbon products of the electrocatalytic CO2 reduction reaction. In such approaches, the CO-generating component of the tandem...

Cited by 25 publications

References 47 publications

Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

The spatial distribution of cobalt phthalocyanine and copper nanocubes controls the selectivity towards C₂ products in tandem electrocatalytic CO₂ reduction

Double‐Dependence Correlations in Graphdiyne‐Supported Atomic Catalysts to Promote CO₂RR toward the Generation of C₂Products

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Tandem electrocatalytic CO2 reduction with Fe-porphyrins and Cu nanocubes enhances ethylene production

Abstract: Copper-based tandem schemes have emerged as promising strategies to promote the formation of multi-carbon products of the electrocatalytic CO2 reduction reaction. In such approaches, the CO-generating component of the tandem...

Cited by 25 publications

References 47 publications

Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

Colloidal-ALD-Grown Metal Oxide Shells Enable the Synthesis of Photoactive Ligand/Nanocrystal Composite Materials

The spatial distribution of cobalt phthalocyanine and copper nanocubes controls the selectivity towards C2 products in tandem electrocatalytic CO2 reduction

Double‐Dependence Correlations in Graphdiyne‐Supported Atomic Catalysts to Promote CO2RR toward the Generation of C2Products

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Product

Resources

About

Tandem electrocatalytic CO₂ reduction with Fe-porphyrins and Cu nanocubes enhances ethylene production

The spatial distribution of cobalt phthalocyanine and copper nanocubes controls the selectivity towards C₂ products in tandem electrocatalytic CO₂ reduction

Double‐Dependence Correlations in Graphdiyne‐Supported Atomic Catalysts to Promote CO₂RR toward the Generation of C₂Products