Nickel (Ni) catalysts supported on mesoporous graphitic carbon nitride (mpg-C3N4) were synthesized through simple impregnation method with air and nitrogen calcination atmosphere for CO methanation. The effects of pretreatment gas on catalyst structure, surface characteristics, and Ni species reducibility were investigated. Under air-calcination condition, the increase in specific surface area of the catalyst can be ascribed to the creation of mesopores and exfoliation of bulk mpg-C3N4 to form thin sheets. However, excessive Ni content on the catalyst accelerated the decomposition of the mpg-C3N4 support during calcination. The catalysts calcined in nitrogen showed lower surface area and fewer number of pores compared to air-treatment. The Ni/mpg-C3N4 catalyst calcined in air with Ni loading 10% exhibited enhanced medium-temperature activity for CO methanation with 79.7% CO conversion and 73.9% CH4 selectivity. This finding can be explained by the formation of mpg-C3N4 thin sheets, which increased the number of catalyst active sites. The CO methanation performance of Ni/mpg-C3N4 catalysts calcined in air was superior to those calcined in nitrogen. Interestingly, CO2 formed by water–gas shift reaction at 320 °C also contributed to the overall methane formation through CO2 methanation. Therefore, mpg-C3N4 thin sheets can be an interesting support for nickel catalyst for CO x methanation.

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.

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The presence of CO2 in gaseous fuel and feedstock stream of chemical reaction was always considered undesirable. High CO2 content will decrease quality and heating value of gaseous fuel, such as biohydrogen, which needs a practical approach to remove it. Thus, this work aims to introduce the first C3N4-metal oxide hybrid for the CO2 cleaning application from a mixture of CO2-H2 gas. The samples were tested for their chemical and physical properties, using field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), physical adsorption analysis (BET), fourier-transform infrared (FTIR), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The CO2 capacity test was carried out by means of a breakthrough test at 1 atm and 25° C using air as a desorption system. Among the samples, amine/metal oxide mass ratio of 2:1 (CNHP500-2(2-1)) showed the best performance of 26.9 wt. % (6.11 mmol/g), with a stable capacity over 6 consecutive cycles. The hybrid sample also showed 3 times better performance than the raw C3N4. In addition, it was observed that the hydrothermal C3N4 synthesis method demonstrated improved chemical properties and adsorption performance than the conventional dry pyrolysis method. In summary, the performance of hybrid samples depends on the different interactive factors of surface area, pore size and distribution, basicity, concentration of amine precursors, ratio of amines precursors to metal oxide, and framework stability.