Summary
Biohydrogen gas is a hot topic for H2 fuel at present. However, removal of the unwanted CO2 through adsorption is required before any system is supplied with high‐purity H2 gas. Herein, we prepared a novel carbon nanoflake hybrid for efficient biohydrogen CO2 capture by combining the advantages of carbon, metal oxide, and amine. Among the samples, SH800 showed a remarkable high CO2 adsorption capacity of 29.8 wt.% (6.77 mmol/g) at 25°C and 1 atm, the highest ever reported at low pressure and temperature. The regeneration experiment also demonstrated robust reversibility over five cycles in the absence of heat treatment. Moreover, it displayed a highly accessible adsorption site with a Brunauer‐Emmett‐Teller (BET) surface area of 600 m2/g and an optimal 6.6‐nm average mesopore structure. Another hybrid named SH500 was also developed. This hybrid showed a comparable CO2 uptake of 27.8 wt.%, being competitive to SH800 but with entirely different chemical properties. Both samples were analyzed by using scanning electron microscopy (SEM), transmission electron microscopy (TEM), BET, Fourier transform infrared spectroscopy (FTIR), X‐ray diffraction (XRD), and X‐ray photoelectron spectroscopy, (XPS) and were tested for CO2 capture through a breakthrough experiment. A highly porous solid adsorbent was also produced via soft‐template synthesis. In summary, the correct amount of dynamic factors, such as high surface area, mesopore‐micropore morphology, activation temperature, metal hybridization, and N moieties, played a major role in the carbon engineering of CO2 adsorbent.