Hydrogenolysis of carbon–oxygen bonds is a versatile synthetic method, of which hydrogenolysis of bioderived 5-hydroxymethylfurfural (HMF) to furanic fuels is especially attractive. However, low-temperature hydrogenolysis (in particular over non-noble catalysts) is challenging. Herein, nickel nanoparticles (NPs) inlaid nickel phyllosilicate (NiSi-PS) are presented for efficient hydrogenolysis of HMF to yield furanic fuels at 130–150 °C, being much superior with impregnated Ni/SiO2 catalysts prepared from the same starting materials. NiSi-PS also shows a 2-fold HMF conversion intrinsic rate and 3-fold hydrogenolysis rate compared with the impregnated Ni/SiO2. The superior performance originated from the synergy of highly dispersed nickel NPs and substantially formed acid sites due to coordinatively unsaturated Ni (II) sites located at the remnant nickel phyllosilicate structure, as revealed by detailed characterizations. The model reactions over the other reference catalysts further highlighted the metal–acid synergy for hydrogenolysis reactions. NiSi-PS can also efficiently catalyze low-temperature hydrogenolysis of bioderived furfural and 5-methylfurfural, demonstrating a great potential for other hydrogenolysis reactions.

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Ethanol synthesis from syngas via dimethyl oxalate (DMO) hydrogenation is of crucial importance for environment- and energy-related applications. Herein, we designed the bifunctional Cu nanoparticle (NP) inlaid mesoporous Al2O3 catalyst and first applied it to ethanol synthesis with high efficiency. The catalyst was made based on the spatial restriction strategy by pinning the Cu NPs on mesoporous Al2O3 to conquer the sintering problem and facilitate the stability (>200 h at 270 °C), which has potential values in high-temperature and exothermic reactions. The plentiful pores, highly exposed and properly assembled Cu-acid sites, furnished the catalyst with high ethanol yield (∼94.9%). A structure-sensitive behavior that the intrinsic activity increases with the decreasing NP size was discussed. It was attributed to the change in metal–acid interfacial sites, morphology, and electronic structure and balance of surface Cu0–Cu+ species. The mechanism for DMO hydrogenation to ethanol involving activation of CO, C–O, and O–H bands was also proposed. As cleavage of these bonds is a versatile tool to utilize bioderived molecules (e.g., polyols), the bifunctional catalysts can also be applied to hydrogenolysis of C–O bonds or etherification of O–H groups to produce various chemicals.

In article number 2001093, Joselito M. Razal and co‐workers demonstrate that ordered domains of additive‐free Ti3C2Tx MXene liquid crystals can be processed into micrometer‐thin films that do not compromise mechanical properties for electrical conductivity, enabling the development of high‐performance devices and new applications.

Low-temperature efficient hydrogenation of CO bonds in various compounds, which is one of the most important processes for producing fuels and chemicals, is of fundamental interest but remains a significant challenge. The primary problem is a lack of heterogeneous catalyst systems that are highly active at ambient or low temperatures. This paper describes an efficient strategy for designing a low-temperature hydrogenation catalyst. Ru nanoparticles supported on reduced graphene oxide (Ru/RGO) show remarkable efficiency for hydrogenation of levulinic acid into γ-valerolactone at temperatures as low as −10 °C. The catalyst is also highly active toward low-temperature hydrogenation of CO bonds in other carbonyl compounds into C−OH bonds, such as furfural, propionaldehyde, 2-pentanone, hydroxyacetone, acetone, acetophenone, cyclohexanone, and benzophenone. X-ray photoelectron spectroscopy and in situ Fourier transform infrared demonstrate that the electron transfer between Ru 0 and RGO leads to the formation of an electron-rich state of Ru 0 nanoparticles that are highly effective for activating CO bonds.