Layered double hydroxides (LDHs) have been considered as promising electrodes for supercapacitors due to their adjustable composition, designable function and superior high theoretic capacity. However, their experimental specific capacity is significantly lower than the theoretical value due to their small interlayer spacing. Therefore, obtaining large interlayer spacing through the intercalation of large‐sized anions is an important means to improve capacity performance. Herein, a metal organic framework derived cobalt‐nickel layered double hydroxide hollowcage intercalated with different concentrations of 1,4‐benzenedicarboxylic acid (H2BDC) through in‐situ cationic etching and organic ligand intercalation method is designed and fabricated. The superior specific capacity and excellent rate performance are benefit from the large specific surface area of the hollow structure and increasing interlayer spacing of LDH after H2BDC intercalation. The sample with the largest layer spacing displays a maximum specific capacity of 229 mA h g−1 at 1 A g−1. In addition, the hybrid supercapacitor assembled from the sample with the largest layer spacing and active carbon electrode has a maximum specific capacity of 158 mA h g−1 at 1 A g−1; the energy density is as high as 126.4 W h kg−1 at 800 W kg−1 and good cycle stability.

Acetylene semihydrogenation is a key technology for producing polymer‐grade ethylene from crude ethylene. Ni‐based catalysts are promising alternatives to noble‐metals for this process. However, achieving high catalytic activity and selectivity remains a big challenge. We report a novel catalyst design based on high‐entropy intermetallics (HEI), which provide thermally stable isolated Ni without excess counterpart metals and achieve exceptionally high performance. Intermetallic NiGa was multi‐metalized to a (NiFeCu)(GaGe), where the Ni and Ga sites were partially substituted with Fe/Cu and Ge, respectively, without altering the parent CsCl‐type structure. The NiFeCuGaGe/SiO2 HEI catalyst completely inhibited ethylene overhydrogenation even at complete acetylene conversion, and exhibited five‐times higher activity than other 3d‐transition‐metal‐based catalysts. The DFT study showed that the surface energy decreased by multi‐metallization, which drastically weakened ethylene adsorption.

The oxidative dehydrogenation of propane using CO2 (CO2-ODP) is a promising technique for high-yield propylene production and CO2 utilization. The development of a highly efficient catalyst for CO2-ODP is of great interest and benefit to the chemical industry as well as net zero emissions. Here, we report a unique catalyst material and design concept based on high-entropy intermetallics for this challenging chemistry. A senary (PtCoNi)(SnInGa) catalyst supported on CeO2 with a PtSn intermetallic structure exhibits a considerably higher catalytic activity, C3H6 selectivity, long-term stability, and CO2 utilization efficiency at 600 °C than previously reported. Multi-metallization of the Pt and Sn sites by Co/Ni and In/Ga, respectively, greatly enhances propylene selectivity, CO2 activation ability, thermal stability, and regenerable ability. The results obtained in this study can promote carbon-neutralization of industrial processes for light alkane conversion.

CO oxidation has attracted great attention in the automobile exhaust treatment and fuel cell industrial process, with Pt as one of the most promising catalysts. The efficiency of the catalyst is still below the requirement of the industry due to limited understanding about the reaction mechanism of CO oxidation by O2 or H2O, which were proposed to be following the similar/same reaction mechanism (the Mars–van Krevelen reaction mechanism). Our recent results indicate that this assumption might not be correct. Here, we design a catalyst with a combination of isolated platinum atoms (Pt1) and nanoparticles (Ptn) supported on MgO-dispersed CeO2−δ (CeO2−δ/MgO), named as 0.5Pt–xCeO2−δ/MgO (x = 0, 1, 2, 5, 10, 20) to establish two types of active sites, one is solely over Pt NPs (type-I) and the other is at the interface between Pt atoms and the reducible metal oxide support CeO2−δ (type-II), and we perform kinetic, thermodynamic, and in situ spectroscopy analysis on this catalyst to prove that CO oxidation by O2 undergoes the Langmuir–Hinshelwood reaction mechanism on type-I sites (Pt NPs), while water–gas shift (WGS) reaction undergoes the Mars–van Krevelen reaction mechanism at the interface between Pt atoms and the reducible support CeO2−δ (type-II) verified by activation energy assessment and the reactant and product pressure dependency studies applied, in which a systematic reduction of the reaction barrier of CO oxidation (by O2) was obtained once the size of Pt NPs increased and was independent of the changes in the size of CeO2−δ, while the reaction barrier of the WGS was very sensitive to the size of CeO2−δ and slightly inert against the size of Pt NPs. Additionally, there is competitive adsorption between CO and O2 over Pt–CeO2−δ/MgO, while there is no competitive adsorption between CO and H2O based on our pressure dependency studies. Collectively, our current work provides convincing evidence that the promotion of H2O on CO oxidation is the change of the reaction mechanism rather than the simple effect of hydroxyl dissociated by H2O dosing.

Acetylene semihydrogenation is a key technology for producing polymer‐grade ethylene from crude ethylene. Ni‐based catalysts are promising alternatives to noble‐metals for this process. However, achieving high catalytic activity and selectivity remains a big challenge. We report a novel catalyst design based on high‐entropy intermetallics (HEI), which provide thermally stable isolated Ni without excess counterpart metals and achieve exceptionally high performance. Intermetallic NiGa was multi‐metalized to a (NiFeCu)(GaGe), where the Ni and Ga sites were partially substituted with Fe/Cu and Ge, respectively, without altering the parent CsCl‐type structure. The NiFeCuGaGe/SiO2 HEI catalyst completely inhibited ethylene overhydrogenation even at complete acetylene conversion, and exhibited five‐times higher activity than other 3d‐transition‐metal‐based catalysts. The DFT study showed that the surface energy decreased by multi‐metallization, which drastically weakened ethylene adsorption.