This study focuses on achieving high photocatalytic activity using MoS/TiO heterostructures (MOT). To this end, MoS and TiO were synthesized by employing hydrothermal synthesis techniques, and then MoS/TiO heterostructures were synthesized by using 1:1, 1:2, 1:3, and 1:4 ratios of MoS and TiO, respectively. While the structural and electronic changes for the 1:2 and 1:3 ratios were relatively minor, significant modifications in bandgaps and morphology were observed for the 1:1 and 1:4 ratios.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Electrocatalytic reduction of NO is a green and sustainable method that not only helps to treat industrial pollutants in wastewater, but also produces valuable chemicals. However, the slow dynamics of the proton-coupled electron transfer process results in a high barrier and low conversion efficiency. In this work, the Se-deficient FeSe/FeO heterojunction was synthesized, which showed excellent electrochemical performance in 0.
View Article and Find Full Text PDFTo mitigate carbon dioxide (CO) emissions and advance carbon neutrality, the conversion of CO into value-added fuels and chemicals via the reverse water-gas shift (RWGS) reaction is recognized as a promising approach. In this study, we designed platinum (Pt)-loaded nitrogen-doped carbon composite dual-phase titanium dioxide (TiO) nanomaterials to achieve efficient photo-thermal performance in the RWGS reaction. The incorporation of Pt, nitrogen doping, and the selection of an appropriate calcination temperature enhance light responsiveness and reduce the recombination of photo-generated carriers, thereby improving the efficiency of the photo-thermal RWGS reaction.
View Article and Find Full Text PDFThe development of efficient electrocatalysts for hydrogen and oxygen evolution reactions (HER and OER) is pivotal for advancing cleaner and sustainable fuel production technologies. The conventional electrocatalysts have limited stability and higher overpotentials, and there is demand to explore advanced materials and synthesis methods. In this context, a novel bifunctional electrocatalyst has been devised through the phosphidation of tungsten molybdenum oxide (P-MoWHO) at relatively low temperatures.
View Article and Find Full Text PDFThe advancement in electrocatalysis, particularly in the development of efficient catalysts for hydrogen and oxygen evolution reactions (HER and OER), is crucial for sustainable energy generation through processes like overall water splitting. A notable bifunctional electrocatalyst, CoFeO/CoFe, has been engineered to facilitate both OER and HER concurrently, aiming to reduce overpotentials. In the pursuit of further enhancing catalytic efficiency, a morphological transformation has been achieved by introducing a sulphur source and multi-walled carbon nanotubes (MWCNTs) into the catalyst system, resulting in S-CoFeO/CoFe/MWCNTs.
View Article and Find Full Text PDFPhoto-thermal co-catalytic reduction of CO to synthesize value-added chemicals presents a promising approach to addressing environmental issues. Nevertheless, traditional catalysts exhibit low light utilization efficiency, leading to the generation of a reduced number of electron-hole pairs and rapid recombination, thereby limiting catalytic performance enhancement. Herein, a Mott-Schottky heterojunction catalyst was developed by incorporating nitrogen-doped carbon coated TiO supported nickel (Ni) nanometallic particles (Ni/x-TiO@NC).
View Article and Find Full Text PDFThe weak adsorption of oxygen on transition metal oxide catalysts limits the improvement of their electrocatalytic oxygen reduction reaction (ORR) performance. Herein, a dopamine-assisted method is developed to prepare Mn-doped ceria supported on nitrogen-doped carbon nanotubes (Mn-Ce-NCNTs). The morphology, dispersion of Mn-doped ceria, composition, and oxygen vacancies of the as-prepared catalysts were analyzed using various technologies.
View Article and Find Full Text PDFSingle-site Fe-N-C catalysts are the most promising Pt-group catalyst alternatives for the oxygen reduction reaction, but their application is impeded by their relatively low activity and unsatisfactory stability as well as production costs. Here, cobalt atoms are introduced into an Fe-N-C catalyst to enhance its catalytic activity by utilizing the synergistic effect between Fe and Co atoms. Meanwhile, phenanthroline is employed as the ligand, which favours stable pyridinic N-coordinated Fe-Co sites.
View Article and Find Full Text PDFDual-atom site catalysts (DASCs) have sparked considerable interest in heterogeneous photocatalysis as they possess the advantages of excellent photoelectronic activity, photostability, and high carrier separation efficiency and mobility. The DASCs involved in these important photocatalytic processes, especially in the photocatalytic hydrogen evolution reaction (HER), CO reduction reaction (CORR), N/nitrate reduction, ., have been extensively investigated in the past few years.
View Article and Find Full Text PDFHydrogen peroxide (HO) is a highly value-added and environmental-friendly chemical with various applications. The production of HO by electrocatalytic 2e oxygen reduction reaction (ORR) has emerged as a promising alternative to the energy-intensive anthraquinone process. High selectivity Catalysts combining with superior activity are critical for the efficient electrosynthesis of HO.
View Article and Find Full Text PDFLignin is the main component of lignocellulose and the largest source of aromatic substances on the earth. Biofuel and bio-chemicals derived from lignin can reduce the use of petroleum products. Current advances in lignin catalysis conversion have facilitated many of progress, but understanding the principles of catalyst design is critical to moving the field forward.
View Article and Find Full Text PDFThe development of highly active and low-cost oxygen reduction reaction (ORR) catalysts is crucial for the practical application of hydrogen fuel cells. However, the linear scaling relation (LSR) imposes an inherent Sabatier's limitation for most catalysts including the benchmark Pt with an insurmountable overpotential ceiling, impeding the development of efficient electrocatalysts. To avoid such a limitation, using earth-abundant metal oxides with different crystal phases as model materials, we propose an effective and dynamic reaction pathway through constructing spatially correlated Pt-Mn pair sites, achieving an excellent balance between high activity and low Pt loading.
View Article and Find Full Text PDFThe development of efficient and economical electrocatalysts for oxygen evolution reaction (OER) is of paramount importance for the sustainable production of renewable fuels and energy storage systems; however, the sluggish OER kinetics involving multistep four proton-coupled electron transfer hampers progress in these systems. Fortunately, surface reconstruction offers promising potential to improve OER catalyst design. Anion modulation plays a crucial role in controlling the extent of surface reconstruction and positively persuading the reconstructed species' performances.
View Article and Find Full Text PDFThe spin degree of freedom is an important and intrinsic parameter in boosting carrier dynamics and surface reaction kinetics of photocatalysis. Here we show that chiral structure in ZnO can induce spin selectivity effect to promote photocatalytic performance. The ZnO crystals synthesized using chiral methionine molecules as symmetry-breaking agents show hierarchical chirality.
View Article and Find Full Text PDFSurface reconstruction generates real active species in electrochemical conditions; rational regulating reconstruction in a targeted manner is the key for constructing highly active catalyst. Herein, we use the high-valence Mo modulated orthorhombic PrIrMoO as model to activate lattice oxygen and cations, achieving directional and accelerated surface reconstruction to produce self-terminated Ir‒O‒Mo (O represents the bridge oxygen) active species that is highly active for acidic water oxidation. The doped Mo not only contributes to accelerated surface reconstruction due to optimized Ir‒O covalency and more prone dissolution of Pr, but also affords the improved durability resulted from Mo-buffered charge compensation, thereby preventing fierce Ir dissolution and excessive lattice oxygen loss.
View Article and Find Full Text PDFThe hydrogen evolution from ammonia borane is intriguing but challenging due to its sluggish kinetics. In this regard, the gold nanoparticles amalgamation with metal phosphides is speculated to be more efficient catalysts. Here, the catalysts Au/NiP and Au/CoP with the high synergetic effect of Au nanoparticles and metal phosphides were synthesized for ammonia borane hydrolysis.
View Article and Find Full Text PDFThe oxygen evolution reaction (OER) severely limits the efficiency of proton exchange membrane (PEM) electrolyzers due to slow reaction kinetics. IrO is currently a commonly used anode catalyst, but its large-scale application is limited due to its high price and scarce reserves. Herein, we reported a practical strategy to construct an acid OER catalyst where Iridium oxide loading and iridium element bulk doping are realized on the surface and inside of WO nanowires by immersion adsorption, respectively.
View Article and Find Full Text PDFDynamic reconstruction of catalyst active sites is particularly important for metal oxide-catalyzed oxygen evolution reaction (OER). However, the mechanism of how vacancy-induced reconstruction aids OER remains ambiguous. Here, we use CoO with Co or O vacancies to uncover the effects of different defects in the reconstruction process and the active motifs relevant to alkaline OER.
View Article and Find Full Text PDFNature-inspired artificial Z-scheme photocatalyst offers great promise in solar overall water splitting, but its rational design, construction and interfacial charge transfer mechanism remain ambiguous. Here, we design an approach of engineering interfacial band bending via work function regulation, which realizes directional charge transfer at interface and affords direct Z-scheme pathway. Taking BiVO as prototype, its oxygen vacancy concentration is reduced by slowing down the crystallization rate, thereby changing the work function from smaller to larger than that of polymeric carbon nitride (PCN).
View Article and Find Full Text PDFThe conversion of biomass is a favorable alternative to the fossil energy route to solve the energy crisis and environmental pollution. As one of the most versatile platform compounds, 5-hydroxymethylfural (HMF) can be transformed to various value-added chemicals via electrolysis combining with renewable energy. Here, the recent advances in electrochemical oxidation of HMF, from reaction mechanism to reactor design are reviewed.
View Article and Find Full Text PDFPhotocatalysis can create a green way to produce clean energy resources, degrade pollutants and achieve carbon neutrality, making the construction of efficient photocatalysts significant in solving environmental issues. Conjugated polymers (CPs) with adjustable band structures have superior light-absorption capacity and flexible morphology that facilitate contact with other components to form advanced heterojunctions. Interface engineering can strengthen the interfacial contact between the components and further enlarge the interfacial contact area, enhance light absorption, accelerate charge transfer and improve the reusability of the composites.
View Article and Find Full Text PDFThe piezo-Fenton system has attracted attention not only because it can enhance the Fenton reaction activity by mechanical energy input, but also because it is expected to realize a class of stimuli-responsive advanced oxidation systems by regulating energy input and hydrogen peroxide self-supply, thus greatly enriching the application possibilities of Fenton chemistry. In this work, a series of Fe-doped g-C N (g-C N -Fe) as a piezo-Fenton system were synthesized where the iron stably immobilized through Fe-N interaction. The piezo-induced electrons generate on g-C N matrix support the conversion of Fe(III) to Fe(II) and promote rate-limiting step of Fenton reaction.
View Article and Find Full Text PDFOne pot synthesis of 2,5-dimethylfuran (2,5-DMF) from saccharides under mild conditions is of importance for the production of biofuel and fine chemicals. However, the synthesis requires a multitude of active sites and suffers from slow kinetics due to poor diffusion in most composite catalysts. Herein, a metal-acid functionalized 2D metal-organic framework (MOF; Pd/NUS-SO H), as an ultrathin nanosheet of 3-4 nm with Lewis acid, Brønsted acid, and metal active sites, was prepared based on the diazo method for acid modification and subsequent metal loading.
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