Ultra-thin (1-3 cationic-layers) (CuZn)1-xGax-CO3 layered double hydroxides (LDH) nanosheets were synthesized following the aqueous miscible organic solvent treatment (AMOST) method and applied as catalyst precursors for methanol production from CO2 hydrogenation. It is found that upon reduction, the aqueous miscible organic solvent treated LDH (AMO-LDH) samples above a critical Ga 3+ composition give consistently and significantly higher Cu surface areas and dispersions than the catalysts prepared from conventional hydroxyl-carbonate phases. Owing to the distinctive local steric and electrostatic stabilization of the ultra-thin LDH structure, the newly formed active Cu(Zn) metal atoms can be stably embedded in the cationic layers, exerting an enhancement to the catalytic reaction. The best catalyst in this study displayed methanol productivity with a space-time yield of 0.6 gMeOH•gcat-1 •h-1 under typical reaction conditions, which as far as we are aware, is higher than most reported Cu-based catalysts in the literature.

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This study employed a novel modification strategy to overcome the intrinsic poor rate performance, large initial irreversible capacity, and low cycling stability of Li-rich layered oxide (LLO) cathode materials. The strategy involved simultaneous in situ spinel Li1+x Ni y Mn2–y O4 coating using Mn-TFBDC (TFBDC: 2,3,5,6-tetrafluoro-1,4-benzenedicarboxylic acid) as the precursor and organic fluorine doping agent. Uniform Li1+x Ni y Mn2–y O4 coating of the LLO surface was easily achieved via the coordination of the carboxylic acid ligands with the manganese ions and subsequent heat treatment. TFBDC-assisted treatment rendered significantly enhanced electrochemical performance to LLO. The first discharge specific capacity of LLO modified by TFBDC-assisted treatment (TA-LLO) was enhanced to 302.1 mAh g–1, and the capacity retention significantly increased from 80.8 to 98.9% after 100 cycles at 1C, compared with that of the pristine LLO (PLLO). Electrochemical impedance spectroscopy and the galvanostatic intermittent titration technique confirmed that TA-LLO had a lower charge transfer resistance and higher ion diffusion coefficient than PLLO. These results suggest that the use of organic fluorine is an effective strategy to carry out fluorine doping simultaneously with spinel Li1+x Ni y Mn2–y O4 coating for fast Li+ ion diffusion and significantly improved electrochemical properties of LLOs.

There is increasing interest in capturing H2 generated from renewables with CO2 to produce methanol. However, renewable hydrogen production is expensive and in limited quantity compared to CO2. Excess CO2 and limited H2 in the feedstock gas is not favorable for CO2 hydrogenation to methanol, causing low activity and poor methanol selectivity. Now, a class of Rh‐In catalysts with optimal adsorption properties to the intermediates of methanol production is presented. The Rh‐In catalyst can effectively catalyze methanol synthesis but inhibit the reverse water‐gas shift reaction under H2‐deficient gas flow and shows the best competitive methanol productivity under industrially applicable conditions in comparison with reported values. This work demonstrates a strong potential of Rh‐In bimetallic composition, from which a convenient methanol synthesis based on flexible feedstock compositions (such as H2/CO2 from biomass derivatives) with lower energy cost can be established.