Faceted Crystal Nanoarchitectonics of Organic–Inorganic 3D-Printed Visible-Light Photocatalysts

Muñoz, José Santiago Álvarez; Rojas, Daniel; Pumera, Martin

doi:10.1021/acsaem.1c03863

Cited by 10 publications

(7 citation statements)

References 58 publications

(82 reference statements)

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“…[119] The reactivity and porosity of the printed product require serious attention. Hence, state-of-the-art works focus [134] on the approach to maximize the photo(electro)catalyst effectiveness whilst unifying them within the polymer matrix. For example, graphene/PLA (G/PLA) polymer is one of the most common filaments used for the FDM process.…”

Section: Fused Deposition Modeling (Fdm)mentioning

confidence: 99%

“…Additionally, Munoz et al reported fabrication of 3Dp graphene/PLA filament by FDM, functionalized with Ag 3 PO 4 nanoarchitectures. [134] Their work has also highlighted activation of commercial G/PLA substrate using DMF prior to catalyst deposition, as to achieve electrically active substrate ready for catalyst deposition. The activated 3Dp substrate was then immersed in Ag 3 PO 4 photoactive material, creating an electrostatic interaction between the Ag ion precursor and the oxygenated groups exposed on G/PLA surface.…”

Section: Fused Deposition Modeling (Fdm)mentioning

confidence: 99%

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Additive Manufacturing: A Paradigm Shift in Revolutionizing Catalysis with 3D Printed Photocatalysts and Electrocatalysts Toward Environmental Sustainability

Khoo,

Ng,

Haw

et al. 2024

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Semiconductor‐based materials utilized in photocatalysts and electrocatalysts present a sophisticated solution for efficient solar energy utilization and bias control, a field extensively explored for its potential in sustainable energy and environmental management. Recently, 3D printing has emerged as a transformative technology, offering rapid, cost‐efficient, and highly customizable approaches to designing photocatalysts and electrocatalysts with precise structural control and tailored substrates. The adaptability and precision of printing facilitate seamless integration, loading, and blending of diverse photo(electro)catalytic materials during the printing process, significantly reducing material loss compared to traditional methods. Despite the evident advantages of 3D printing, a comprehensive compendium delineating its application in the realm of photocatalysis and electrocatalysis is conspicuously absent. This paper initiates by delving into the fundamental principles and mechanisms underpinning photocatalysts electrocatalysts and 3D printing. Subsequently, an exhaustive overview of the latest 3D printing techniques, underscoring their pivotal role in shaping the landscape of photocatalysts and electrocatalysts for energy and environmental applications. Furthermore, the paper examines various methodologies for seamlessly incorporating catalysts into 3D printed substrates, elucidating the consequential effects of catalyst deposition on catalytic properties. Finally, the paper thoroughly discusses the challenges that necessitate focused attention and resolution for future advancements in this domain.

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Section: Fused Deposition Modeling (Fdm)mentioning

confidence: 99%

Section: Fused Deposition Modeling (Fdm)mentioning

confidence: 99%

Additive Manufacturing: A Paradigm Shift in Revolutionizing Catalysis with 3D Printed Photocatalysts and Electrocatalysts Toward Environmental Sustainability

Khoo,

Ng,

Haw

et al. 2024

Small

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“…Up to date, inorganic semiconductors have been mainly used for designing 3D‐printed photocatalysts with applications in energy and environmental remediation [8] . However, the lack of solubility of such materials in organic solvents results in an inhomogeneous dispersion of the photocatalytic nanoparticles in the thermoplastics that complicates the whole fabrication and extrusion process.…”

Section: Introductionmentioning

confidence: 99%

“…[6c,7] Up to date, inorganic semiconductors have been mainly used for designing 3D-printed photocatalysts with applications in energy and environmental remediation. [8] However, the lack of solubility of such materials in organic solvents results in an inhomogeneous dispersion of the photocatalytic nanoparticles in the thermoplastics that complicates the whole fabrication and extrusion process. Here, we present the design of a 3Dprinted hierarchical porous structure, containing an organic photoactive molecule (EBE), based on a conjugated trimer with a DÀ AÀ D configuration (4,7-bis(thieno[3,4-b][1,4]dioxin-5yl)benzo[c][1,2,5]thiadiazole), for the photocatalytic degradation of persistent organic pollutants and hydrogen generation.…”

Section: Introductionmentioning

confidence: 99%

3D‐Printed Organic Conjugated Trimer for Visible‐Light‐Driven Photocatalytic Applications

et al. 2023

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Small molecule organic semiconductors (SMOSs) have emerged as a new class of photocatalysts that exhibit visible light absorption, tunable bandgap, good dispersion, and solubility. However, the recovery and reusability of such SMOSs in consecutive photocatalytic reactions is challenging. This work concerns a 3D-printed hierarchical porous structure based on an organic conjugated trimer, named EBE. Upon manufacturing, the photophysical and chemical properties of the organic semiconductor are maintained. The 3D-printed EBE photocatalyst shows a longer lifetime (11.7 ns) compared to the powder-state EBE (1.4 ns). This result indicates a microenvironment effect of the solvent (acetone), a better dispersion of the catalyst in the sample, and reduced intermolecular πÀ π stacking, which results in improved separation of the photo-generated charge carriers. As a proof-of-concept, the photocatalytic activity of the 3D-printed EBE catalyst is evaluated for water treatment and hydrogen production under sun-like irradiation. The resulting degradation efficiencies and hydrogen generation rates are higher than those reported for the state-ofthe-art 3D-printed photocatalytic structures based on inorganic semiconductors. The photocatalytic mechanism is further investigated, and the results suggest that hydroxyl radicals (HO * ) are the main reactive radicals responsible for the degradation of organic pollutants. Moreover, the recyclability of the EBE-3D photocatalyst is demonstrated in up to 5 uses. Overall, these results indicate the great potential of this 3Dprinted organic conjugated trimer for photocatalytic applications.

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“…[31][32][33] Recently, various studies have demonstrated the suitability of physically interacting CDs with some inorganic-based 2D materials, such as transition-metal carbides, [34] dichalcogenides, [35] and oxides, [36] to provide unique organicinorganic 0D/2D nanoarchitectonics with enhanced and even new physicochemical characteristics. [37][38][39] Further, calculation studies have shown the benefits of combining germanene and SiC layers to tune the electronic properties of Ge-based derivatives. [40] Consequently, engineering robust organic-inorganic 2D-Ge heterostructures employing covalent chemistry would be a fruitful path toward devising advanced 2D-Ge materials/ devices for task-specific applications.…”

Section: Introductionmentioning

confidence: 99%

Synthetic Nanoarchitectonics of Functional Organic–Inorganic 2D Germanane Heterostructures via Click Chemistry

et al. 2022

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counterparts, resulting in outstanding physicochemical characteristics.Concretely, germanene (the germanium analog of mainstream graphene) and its saturated forms-obtained by topochemical deintercalation of bulkier Ca 2 Ge into 2D germanane (2D-Ge) derivatives where each Ge atom is covalently bonded to a terminal ligand (e.g., H, CH 3 , or CH 2 CHCH 2 )-have recently attracted particular attention since they exhibit similar promising electronic features to graphene. [15][16][17] In addition, the fact that its bandgap can be easily modulated by tailoring the tethered terminal ligand has further stimulated interest in the synthesis of 2D-Ge derivatives, which present themselves as ideal candidates for a variety of (opto)electronic tasks, including bio-sensing, energy storage and conversion, catalysis, and beyond. [4,[18][19][20][21] Albeit being a very promising material, the vast majority of works involving 2D-Ge derivatives are mainly focused on either developing computational studies or discussing fundamental aspects, with minimum emphasis on their experimental implementation. [21,22] Consequently, there is enough room for realizing functional 2D-Ge-based materials/devices and their exploration for specific achievements.To date, the combination of organic and inorganic nanomaterials has led to the creation of unique heterostructuresreferred to as architectures composed of more than one Succeeding graphene, 2D inorganic materials made of reactive van der Waals layers, like 2D germanane (2D-Ge) derivatives, have attracted great attention because their physicochemical characteristics can be entirely tuned by modulating the nature of the surface substituent. Although very interesting from a scientific point of view, almost all the reported works involving 2D-Ge derivatives are focused on computational studies. Herein, a first prototype of organic-inorganic 2D-Ge heterostructure has been synthesized by covalently anchoring thiol-rich carbon dots (CD-SH) onto 2D allyl germanane (2D-aGe) via a simple and green "one-pot" click chemistry approach. Remarkably, the implanted characteristics of the carbon nanomaterial provide new physicochemical features to the resulting 0D/2D heterostructure, making possible its implementation in yet unexplored optoelectronic tasks-e.g., as a fluorescence resonance energy transfer (FRET) sensing system triggered by supramolecular π-π interactions-that are inaccessible for the pristine 2D-aGe counterpart. Consequently, this work builds a foundation toward the robust achievement of functional organic-inorganic 2D-Ge nanoarchitectonics through covalently assembling thiol-rich carbon nanoallotropes on commercially available 2D-aGe.

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Faceted Crystal Nanoarchitectonics of Organic–Inorganic 3D-Printed Visible-Light Photocatalysts

Cited by 10 publications

References 58 publications

Additive Manufacturing: A Paradigm Shift in Revolutionizing Catalysis with 3D Printed Photocatalysts and Electrocatalysts Toward Environmental Sustainability

Additive Manufacturing: A Paradigm Shift in Revolutionizing Catalysis with 3D Printed Photocatalysts and Electrocatalysts Toward Environmental Sustainability

3D‐Printed Organic Conjugated Trimer for Visible‐Light‐Driven Photocatalytic Applications

Synthetic Nanoarchitectonics of Functional Organic–Inorganic 2D Germanane Heterostructures via Click Chemistry

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