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Photoassisted methanation using Cu2O nanoparticles supported on graphene as a photocatalyst

机译:使用负载在石墨烯上的Cu2O纳米粒子作为光催化剂进行光辅助甲烷化

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摘要

Photoassisted CO2 methanation can be carried out efficiently at 250 degrees C using Cu2O nanoparticles supported on few layer graphene (Cu2O/G) as a photocatalyst. The Cu2O/G photocatalyst has been prepared by chemical reduction of a Cu salt (Cu(NO3)(2)) with ethylene glycol in the presence of defective graphene obtained from the pyrolysis of alginic acid at 900 degrees C under Ar flow. Using this photocatalyst a maximum specific CH4 formation rate of 14.93 mmol g(Cu2O)(-1) h(-1) and an apparent quantum yield of 7.84% were achieved, which are among the highest reported values for the gas-phase methanation reaction at temperatures below the Sabatier reaction temperature (4350 degrees C). It was found that the most probable reaction mechanism involves photoinduced electron transfer from the Cu2O/G photocatalyst to CO2, while evidence indicates that light-induced local temperature increase and H-2 activation are negligible. The role of the temperature in the process has been studied, the available data suggesting that heating is needed to desorb the H2O formed as the product during the methanation. The most probable reaction mechanism seems to follow a dissociative pathway involving detachment of oxygen atoms from CO2.
机译:使用负载在几层石墨烯上的Cu2O纳米颗粒(Cu2O / G)作为光催化剂,可以在250摄氏度下有效地进行光辅助CO2甲烷化。 Cu2O / G光催化剂的制备方法是,在有缺陷的石墨烯存在下,用乙二醇对铜盐(Cu(NO3)(2))进行化学还原,而该石墨烯是从藻酸在Ar气流中于900℃下热解获得的。使用这种光催化剂,可获得的最大比CH4生成速率为14.93 mmol g(Cu2O)(-1)h(-1)和表观量子产率为7.84%,这是气相甲烷化反应报告的最高值温度低于Sabatier反应温度(4350摄氏度)。发现最可能的反应机理涉及光诱导的电子从Cu2O / G光催化剂转移到CO2,而证据表明光诱导的局部温度升高和H-2活化可忽略不计。已经研究了温度在该过程中的作用,现有数据表明需要加热以解吸甲烷化过程中作为产物形成的H2O。最可能的反应机制似乎遵循一种离解途径,该过程涉及氧原子与二氧化碳的分离。

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