Highly stable and active catalysts are of significant importance and a longstanding challenge for a number of industrial chemical transformations. Here, motivated by the principle of the high entropy-stabilized structure, high-entropy alloy-loaded porous TiO as an efficient and sintering-resistant catalyst for the light-driven reverse water gas‒shift reaction without external heating is synthesized. The optimized CoNiCuPdRu/TiO catalyst exhibits a long-term stability of 1000 h (1.
View Article and Find Full Text PDFDry reforming of methane (DRM) is a promising technique for converting greenhouse gases (namely, CH and CO) into syngas. However, traditional thermocatalytic processes require high temperatures and suffer from low selectivity and coke-induced instability. Here, we report high-entropy alloys loaded on SrTiO as highly efficient and coke-resistant catalysts for light-driven DRM without a secondary source of heating.
View Article and Find Full Text PDFLight-driven hydrogenation of nitro compounds to functionalized amines is of great importance yet a challenge for practical applications, which calls for the development of high-performance, nonprecious photocatalysts and efficient catalytic systems. Herein, we report a high-efficiency FeO@TiO photocatalyst via a sol-gel and subsequent pyrolysis strategy, which exhibits desirable photothermal hydrogenation performance of nitro compounds to functionalized amines with the excellent selectivity of >90% exceeding those of the state-of-the-art heterogeneous photocatalysts. Our experimental results and theoretical calculations for the first time reveal that FeO is the major active phase, and the strong metal-support interaction between FeO and reducible TiO further leads to performance improvement, taking advantage of the enhanced photothermal effect and the improved adsorption for the reactant and hydrazine hydrate.
View Article and Find Full Text PDFImitating the natural photosynthesis to synthesize hydrocarbon fuels represents a viable strategy for solar-to-chemical energy conversion, where utilizing low-energy photons, especially near-infrared photons, has been the ultimate yet challenging aim to further improving conversion efficiency. Plasmonic metals have proven their ability in absorbing low-energy photons, however, it remains an obstacle in effectively coupling this energy into reactant molecules. Here we report the broadband plasmon-induced CO reduction reaction with water, which achieves a CH production rate of 0.
View Article and Find Full Text PDFPhotocatalysis is a promising yet challenging approach for the selective oxidation of hydrocarbons to valuable oxygenated chemicals with O under mild conditions. In this work, we report an atomically precise material model to address this challenge. The key to our solution is the rational incorporation of Fe species into polyoxotitanium cluster to form a heterometallic Ti Fe cocrystal.
View Article and Find Full Text PDFPhotocatalysis under mild conditions is an intriguing avenue for organic chemical manufacturing to confront the serious fossil energy crisis. Herein, we report a direct light-driven alkene production through alcohol dehydration, using nonstoichiometric tungsten oxide of WO nanowires with abundant lattice defects as a photocatalyst. A representative ethylene (CH) production rate of 275.
View Article and Find Full Text PDFTo avoid the energy-consuming step of direct N≡N bond cleavage, photocatalytic N fixation undergoing the associative pathways has been developed for mild-condition operation. However, it is a fundamental yet challenging task to gain comprehensive understanding on how the associative pathways (i.e.
View Article and Find Full Text PDFExploring the advanced oxygen evolution reaction (OER) electrocatalysts is highly desirable toward sustainable energy conversion and storage, yet improved efficiency in acidic media is largely hindered by its sluggish reaction kinetics. Herein, we rationally manipulate the electronic states of the strongly electron correlated pyrochlore ruthenate YRuO alternative through partial A-site substitution of Sr for Y, efficiently improving its intrinsic OER activity. The optimized YSrRuO candidate observes a highly intrinsic mass activity of 1018 A g at an overpotential of 300 mV with excellent durability in 0.
View Article and Find Full Text PDFNitrogen fixation in a simulated natural environment (i.e., near ambient pressure, room temperature, pure water, and incident light) would provide a desirable approach to future nitrogen conversion.
View Article and Find Full Text PDFTwo-dimensional g-C3N4 nanosheets with few-layer thickness, ensuring equivalent charge migrations to various Pd facets, provide an ideal model system for reliably examining the facet selectivity of Pd co-catalysts. It reveals that reduction of CO2 can occur better on Pd{111} facets while H2O prefers to generate H2 on Pd{100}.
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