Highly dispersed bimetallic Pd-In catalysts on Al 2 O 3 were prepared by a simple impregnation method. In comparison with the unsupported intermetallic catalyst, the supported Pd-In catalyst exhibited several magnitudes higher activity and similar selectivity for selective acetylene hydrogenation. Moreover, the activity, selectivity, and anticoking performance of the Pd-In catalyst were superior to those of the monometallic Pd catalyst. The electron transferred from indium weakened the adsorption of ethylene on the negatively charged Pd sites and hence improved the selectivity of Pd-In/Al 2 O 3 . The inhibited formation of hydride due to the presence of indium also contributed to the higher selectivity. The promoted activation of hydrogen, owing to the weak adsorption of acetylene on Pd-In/Al 2 O 3 , and decreased particle size jointly contributed to the enhanced activity of Pd-In/Al 2 O 3 . In addition, green oil formation on Pd-In/Al 2 O 3 was retarded by the presence of indium, contributing to the enhanced stability of the catalyst. The bimetallic Pd-In catalysts showed a strongly composition dependent performance, which resulted from the different extent of electronic and/or geometric modification of Pd active sites.

Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory‐guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi‐hydrogenation processes. Such Ni sites show not only preferential acetylene π‐adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration‐corrected high‐resolution scanning transmission electron microscopy and X‐ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi‐atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.

Critical barriers to layered Ni-rich cathode commercialisation include their rapid capacity fading and thermal runaway from crystal disintegration and their interfacial instability. Structure combines surface modification is the ultimate choice to overcome these. Here, a synchronous gradient Al-doped and LiAlO2-coated LiNi0.9Co0.1O2 cathode is designed and prepared by using an oxalate-assisted deposition and subsequent thermally driven diffusion method. Theoretical calculations, in situ X-ray diffraction results and finite-element simulation verify that Al3+ moves to the tetrahedral interstices prior to Ni2+ that eliminates the Li/Ni disorder and internal structure stress. The Li+-conductive LiAlO2 skin prevents electrolyte penetration of the boundaries and reduces side reactions. These help the Ni-rich cathode maintain a 97.4% cycle performance after 100 cycles, and a rapid charging ability of 127.7 mAh g−1 at 20 C. A 3.5-Ah pouch cell with the cathode and graphite anode showed more than a 500-long cycle life with only a 5.6% capacity loss.