Harnessing inexhaustible solar energy for CO valorization is a substantial step toward achieving a carbon-neutral energy cycle. However, CO conversion often exhibits slow kinetics, necessitating the utilization of sacrificial agents making the process economically unfeasible. In the ongoing quest for sustainable and economically feasible CO valorization, herein the photoreduction of CO to CO coupled with biomass-based alcohol oxidation to fine chemicals is reported via BiWO/g-CN (BWO/g-CN) 2D-2D nanosheet based S-scheme heterojunction.
View Article and Find Full Text PDFThe possibility of converting waste plastics into carbon dots (CDs) with 100% efficiencies using KMnO has emerged as a significant discovery in mitigating plastic pollution and upcycling. However, the lack of tunability of their properties, viz. aerial O harvesting, light-induced autophagy, and photoactivity using air as a free oxidant, has remained a bottleneck.
View Article and Find Full Text PDFHybrid halide perovskites (HHPs), whose every branch generates intrusiveness, have been utilized in solar cells from a broader perspective. However, the inclusiveness of employing HHP as a photocatalyst is in its initial stage. This study mainly focuses on the unexpected utilization of, so far, undesirable material vacancy-ordered MASnBr quantum dots synthesized from MASnBr nanosheets.
View Article and Find Full Text PDFAchieving a high electrocatalytic performance using a completely metal-free electrocatalyst, preferably based on only carbonaceous materials, remains a challenge. Alternatively, an efficient composite of a carbon nanostructure and a non-noble metal with minimum dependence on a metal holds immense potential. Although single-atom catalysis brings superior performance, its complex synthetic strategy limits its large-scale implementation.
View Article and Find Full Text PDFIn recent years, due to high energy consumption in the building sector and subsequent environmental issues, environment-friendly and cost-effective thermally insulating materials are in high demand to improve the energy efficiency of buildings. Current commercially available thermal insulating materials (polystyrene) always pose a challenge due to their non-biodegradability and poor insulating performance. To this end, biomass-derived aerogels are attracting significant interest as renewable and sustainable insulating materials.
View Article and Find Full Text PDFThe selective conversion of 5-hydroxymethyfurfural (HMF), a biomass-derived platform molecule, to value added chemicals can ease the burden on petroleum-based fine chemical synthesis. The active contribution of renewable energy sources along with low cost, environmental friendliness, and a simple reaction system must be adopted for better sustainability. In this context, photocatalytic selective hydrogenation of HMF to 2,5-bis(hydroxymethyl)furan (BHMF) was achieved over P25 titania nanoparticles without chemical squander.
View Article and Find Full Text PDFDisintegrable inorganic nanoclusters (GIONs) with gold seed (GS) coating of an iron oxide core with a primary nanoparticle size less than 6 nm were prepared for theranostic applications. The GIONs possessed a broad near-infrared (NIR) absorbance at ∼750 nm because of plasmon coupling between closely positioned GSs on the iron oxide nanoclusters (ION) surface, in addition to the ∼513 nm peak corresponding to the isolated GS. The NIR laser-triggered photothermal response of GIONs was found to be concentration-dependent with a temperature rise of ∼8.
View Article and Find Full Text PDFInorganic nanomaterials require optimal engineering to retain their functionality yet can also biodegrade within physiological conditions to avoid chronic accumulation in their native form. In this work, we have developed gelatin-stabilized iron oxide nanoclusters having a primary crystallite size of ∼10 nm and surface-functionalized with indocyanine green (ICG)-bound albumin-stabilized gold nanoclusters (Prot-IONs). The Prot-IONs are designed to undergo disintegration in an acidic microenvironment of tumor in the presence of proteolytic enzymes within 72 h.
View Article and Find Full Text PDFGraphitic carbon nitride (also known as g-CN or g-CN) has the intrinsic ability to generate electron-hole pairs under visible light illumination, resulting in the generation of reactive oxygen species (ROS). We report g-CN quantum dots (g-CNQDs) as a standalone photodynamic transducer for imparting significant oxidative stress in glioma cells, manifested by the loss of mitochondrial membrane potential. With an optimized treatment time, visible light source, and exposure window, the photodynamic treatment with g-CNQDs could achieve ∼90% cancer cell death via apoptosis.
View Article and Find Full Text PDFThe capture and catalytic conversion of CO into value-added chemicals is a promising and sustainable approach to tackle the global warming and energy crisis. The nitrogen-rich porous organic polymers are excellent materials for CO capture and separation. Herein, we present a nitrogen-rich heptazine-based microporous polymer for the cycloaddition reaction of CO with epoxides in the absence of metals and solvents.
View Article and Find Full Text PDFA heptazine-based microporous polymeric network, HMP-TAPA was synthesised by direct coupling of trichloroheptazine and tris(4-aminophenyl)amine (TAPA). A high surface area of 424 m /g was achieved, which is the highest surface area among heptazine-based polymeric networks (HMPs). The tailored electron-donor and -acceptor units in HMP-TAPA give broad visible-light absorption.
View Article and Find Full Text PDFThe emerging class of heptazine-based polymeric materials has shown potential candidature as photocatalyst materials for hydrogen evolution. At the same time, they have shown promising application as solid base materials to catalyse various organic transformations. Thus, the material design rationale needs to be developed around the heptazine-based polymeric frameworks in order to specifically design task specific materials.
View Article and Find Full Text PDFMetal-free organic polymer photocatalysts have attracted dramatic attention in the field of visible light-induced hydrogen evolution reaction (HER). Herein, we showed a polymeric O-linked heptazine polymer (OLHP) decorated with S, N co-doped graphene quantum dots (S,N-GQDs) as a photosensitizer to generate hydrogen upon quantum dot sensitization. Both of these heptazine-based systems show effective photosensitization with strong π-π interactions and enhanced photocatalytic H generation (24 times) as metal-free systems.
View Article and Find Full Text PDFA mesoporous magnetic nanohybrid functionalized with 14 wt % carbon nitride (CN) and loaded with curcumin (Cur) has been developed as a combination platform for photodynamic therapy and magnetic hyperthermia. CN-Cur complexes on the nanoparticle surface facilitate fast charge separation of hole-electron pairs under blue LED light irradiation and subsequent singlet oxygen generation. Cur release from the nanoparticle was significant only when exposed to both lysosomal pH (pH = 5.
View Article and Find Full Text PDFLiquid phase adsorption is a common technique in waste water purification. However, this process has some downsides. The removal of environmentally harmful contaminants from organic liquids by adsorption produces secondary waste which has to be treated afterwards.
View Article and Find Full Text PDFA new class of hydrogen (H) bonded fluorescent liquid crystals (FLCs) based on a newly discovered s-heptazine fluorophore discotic component have been synthesized. The tendency of the s-heptazine core to form H-bonded LCs has been explored for the first time. Interestingly, the pure heptazine derivatives (non-mesomorphic) on complexation with tri-alkoxy benzoic acids exhibit enantiotropic columnar mesomorphism over a wide range of temperatures including room temperature.
View Article and Find Full Text PDFHerein, room-temperature discotic liquid crystals based on heptazine, an electron deficient central core, are reported for the first time. Mesomorphic behaviors of the materials are also investigated. Supramolecular assembly of the mesophase derivatives were confirmed by X-ray scattering experiments.
View Article and Find Full Text PDFDevelopment of room-temperature gas sensors is a much sought-after aspect that has fostered research in realizing new two-dimensional materials with high surface area for rapid response and low-ppm detection of volatile organic compounds (VOCs). Herein, a fast-response and low-ppm ethanol gas sensor operating at near room temperature has been fabricated successfully by utilizing cubic mesoporous graphitic carbon nitride (g-CN, commonly known as g-CN), synthesized through template inversion of mesoporous silica, KIT-6. Upon exposure to 50 ppm ethanol at 250 °C, the optimized Ag/g-CN showed a significantly higher response ( / = 49.
View Article and Find Full Text PDFThe fabrication of highly responsive, rapid response/recovery and durable relative humidity (%RH) sensors that can precisely monitor humidity levels still remains a considerable challenge for realizing the next generation humidity sensing applications. Herein, we report a remarkably sensitive and rapid %RH sensor having a reversible response using a nanocasting route for synthesizing mesoporous g-CN (commonly known as g-CN). The 3D replicated cubic mesostructure provides a high surface area thereby increasing the adsorption, transmission of charge carriers and desorption of water molecules across the sensor surfaces.
View Article and Find Full Text PDFHerein, we present an approach to create a hybrid between single-atom-dispersed silver and a carbon nitride polymer. Silver tricyanomethanide (AgTCM) is used as a reactive comonomer during templated carbon nitride synthesis to introduce both negative charges and silver atoms/ions to the system. The successful introduction of the extra electron density under the formation of a delocalized joint electronic system is proven by photoluminescence measurements, X-ray photoelectron spectroscopy investigations, and measurements of surface ζ-potential.
View Article and Find Full Text PDFCharge transport in polymeric graphitic carbon nitrides is shown to proceed via diffusive hopping of electron and hole polarons with reasonably high mobilities >10(-5) cm(2) V(-1) s(-1). The power-law behavior of the ultrafast luminescence decay exhibits that the predominant transport direction is perpendicular to the graphitic polymer sheets, thus complementing 2D materials like graphene.
View Article and Find Full Text PDFThe nature of a nickel-based co-catalyst deposited on a sol-gel prepared porous graphitic-carbon nitride (sg-CN), for photocatalytic H2 production from water, has been investigated. The formation of the active catalytic species, charge separation and recombination of the photogenerated electrons and holes during photochemical H2 evolution has been determined for the first time using in situ EPR spectroscopy.
View Article and Find Full Text PDFComposites of mesoporous polymeric carbon nitride and tungsten(VI) oxide show very high photocatalytic activity for the evolution of hydrogen from water under visible light and in the presence of sacrificial electron donors. Already addition of very small amounts of WO3 yields up to a twofold increase in the efficiency when compared to bulk carbon nitrides and their composites and more notably even to the best reported mesoporous carbon nitride-based photocatalytic materials. The higher activity can be attributed to the high surface area and synergetic effect of the carbon nitrides and the WO3 resulting in improved charge separation through a photocatalytic solid-state Z-scheme mechanism.
View Article and Find Full Text PDFNickel-manganese oxides with variable Ni : Mn ratios, synthesised from heterobimetallic single-source precursors, turned out to be efficient water oxidation catalysts. They were subjected to oxidant-driven, photo- and electro-catalytic water oxidation showing superior activity and remarkable stability. In addition, a structure-activity relation could be established.
View Article and Find Full Text PDFTwo emerging material classes are combined in this work, namely polymeric carbon nitrides and microporous polymer networks. The former, polymeric carbon nitrides, are composed of amine-bridged heptazine moieties and showed interesting performance as a metal-free photocatalyst. These materials have, however, to be prepared at high temperatures, making control of their chemical structure difficult.
View Article and Find Full Text PDF