Experimental and Computational Investigation of CO 2 Capture on Mix-ligand Metal-organic Framework UiO-66

Huang, Qianru; Ding, Jing; Huang, Xiang; Wei, Xiaolan; Wang, Weilong

doi:10.1016/j.egypro.2017.03.933

Cited by 23 publications

(10 citation statements)

References 8 publications

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Section: Discussionsupporting

confidence: 71%

“…Noteworthy is that ReRu-66-NH2(R 2.1) shows markedly higher uptake than ReRu-66(R 2.1), despite comparable N2 adsorption isotherms (Figures 5b and S2). This has been previously observed and attributed to interactions/reactions between the polar linkers' amine groups and carbon dioxide (Figure 5c) [57,58]. Thus, 66-NH2 provides an increased local CO2 concentration available during the course of photocatalysis, thereby reducing diffusion limitations, as well as potentially As photocatalysis proceeds in colloidal solution, the local CO 2 concentration available for catalyst centers could impact the final activity.…”

Section: Discussionmentioning

confidence: 55%

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Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Stanley

Warnan

2021

Energies

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Colloidal dye-sensitized photocatalysis is a promising route toward efficient solar fuel production by merging properties of catalysis, support, light absorption, and electron mediation in one. Metal-organic frameworks (MOFs) are host materials with modular building principles allowing scaffold property tailoring. Herein, we combine these two fields and compare porous Zr-based MOFs UiO-66-NH2(Zr) and UiO-66(Zr) to monoclinic ZrO2 as model colloid hosts with co-immobilized molecular carbon dioxide reduction photocatalyst fac-ReBr(CO)3(4,4′-dcbpy) (dcbpy = dicarboxy-2,2′-bipyridine) and photosensitizer Ru(bpy)2(5,5′-dcbpy)Cl2 (bpy = 2,2′-bipyridine). These host-guest systems demonstrate selective CO2-to-CO reduction in acetonitrile in presence of an electron donor under visible light irradiation, with turnover numbers (TONs) increasing from ZrO2, to UiO-66, and to UiO-66-NH2 in turn. This is attributed to MOF hosts facilitating electron hopping and enhanced CO2 uptake due to their innate porosity. Both of these phenomena are pronounced for UiO-66-NH2(Zr), yielding TONs of 450 which are 2.5 times higher than under MOF-free homogeneous conditions, highlighting synergistic effects between supramolecular photosystem components in dye-sensitized MOFs.

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Section: Discussionsupporting

confidence: 71%

Section: Discussionmentioning

confidence: 55%

Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Stanley

Warnan

2021

Energies

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“…Herein, we report a photoinduction method (PIM) to construct isolated Cu SAs (as active species) anchored on UiO-66-NH 2 (powerful CO 2 enrichment support) − as a robust photocatalyst (Cu SAs/UiO-66-NH 2 ) toward the conversion of CO 2 to liquid fuels. Confined and coordinated Cu SAs species were captured by −NH 2 groups of UiO-66-NH 2 support and then anchored after irradiation with visible light, which optimized the structure of photocatalysts at the atomic level to facilitate the separation of electron–hole pairs.…”

Section: Introductionmentioning

confidence: 99%

Photoinduction of Cu Single Atoms Decorated on UiO-66-NH₂ for Enhanced Photocatalytic Reduction of CO₂ to Liquid Fuels

et al. 2020

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Photocatalytic reduction of CO 2 to value-added fuels is a promising route to reduce global warming and enhance energy supply. However, poor selectivity and low efficiency of catalysts are usually the limiting factor of their applicability. Herein, a photoinduction method was developed to achieve the formation of Cu single atoms on a UiO-66-NH 2 support (Cu SAs/UiO-66-NH 2 ) that could significantly boost the photoreduction of CO 2 to liquid fuels. Notably, the developed Cu SAs/UiO-66-NH 2 achieved the solar-driven conversion of CO 2 to methanol and ethanol with an evolution rate of 5.33 and 4.22 μmol h −1 g −1 , respectively. These yields were much higher than those of pristine UiO-66-NH 2 and Cu nanoparticles/UiO-66-NH 2 composites. Theoretical calculations revealed that the introduction of the Cu SAs on the UiO-66-NH 2 greatly facilitates the conversion of CO 2 to CHO* and CO* intermediates, leading to excellent selectivity toward methanol and ethanol. This study provides new insights for designing high-performance catalyst for photocatalytic reduction of CO 2 at the atomic scale.

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“…Due to their large capacity for the adsorption of gases and structural and chemical tenability, they have gained much attention to the potential applications of CO 2 capture [ 1 , 2 ]. The UiO-66 sample with good thermal stability (>500 °C) and water resistance shows some improved CO 2 adsorption performance [ 3 , 4 , 5 ]. Moreover, when compared with the performance of industrial adsorbent (zeolite 13x, for example), the adsorption capacity of UiO-66 demonstrates an improved value [ 1 , 6 ].…”

Section: Introductionmentioning

confidence: 99%

UiO-66-NH2/GO Composite: Synthesis, Characterization and CO2 Adsorption Performance

et al. 2018

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In this work, a new composite materials of graphene oxide (GO)-incorporated metal-organic framework (MOF)(UiO-66-NH2/GO) were in-situ synthesized, and were found to exhibit enhanced high performances for CO2 capture. X-ray diffraction (XRD), scanning electron microscope (SEM), N2 physical adsorption, and thermogravimetric analysis (TGA) were applied to investigate the crystalline structure, pore structure, thermal stability, and the exterior morphology of the composite. We aimed to investigate the influence of the introduction of GO on the stability of the crystal skeleton and pore structure. Water, acid, and alkali resistances were tested for physical and chemical properties of the new composites. CO2 adsorption isotherms of UiO-66, UiO-66-NH2, UiO-66/GO, and UiO-66-NH2/GO were measured at 273 K, 298 K, and 318 K. The composite UiO-66-NH2/GO exhibited better optimized CO2 uptake of 6.41 mmol/g at 273 K, which was 5.1% higher than that of UiO-66/GO (6.10 mmol/g). CO2 adsorption heat and CO2/N2 selectivity were then calculated to further evaluate the CO2 adsorption performance. The results indicated that UiO-66-NH2/GO composites have a potential application in CO2 capture technologies to alleviate the increase in temperature of the earth’s atmosphere.

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Experimental and Computational Investigation of CO 2 Capture on Mix-ligand Metal-organic Framework UiO-66

Cited by 23 publications

References 8 publications

Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Photoinduction of Cu Single Atoms Decorated on UiO-66-NH₂ for Enhanced Photocatalytic Reduction of CO₂ to Liquid Fuels

UiO-66-NH2/GO Composite: Synthesis, Characterization and CO2 Adsorption Performance

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Experimental and Computational Investigation of CO 2 Capture on Mix-ligand Metal-organic Framework UiO-66

Cited by 23 publications

References 8 publications

Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production

Photoinduction of Cu Single Atoms Decorated on UiO-66-NH2 for Enhanced Photocatalytic Reduction of CO2 to Liquid Fuels

UiO-66-NH2/GO Composite: Synthesis, Characterization and CO2 Adsorption Performance

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Product

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Photoinduction of Cu Single Atoms Decorated on UiO-66-NH₂ for Enhanced Photocatalytic Reduction of CO₂ to Liquid Fuels