Activity of La0.75Sr0.25Cr0.5Mn0.5O3?δ, Ni3Sn2 and Gd-doped CeO2 towards the reverse water-gas shift reaction and carburisation for a high-temperature H2O/CO2 co-electrolysis

摘要

The syngas mixture of CO and H _(2) , e.g. from natural gas reforming, is currently an important feedstock supplier for the synthesis of numerous chemicals. In order to minimize fossil source dependency and reduce global warming, alternative processes to produce syngas, such as high-temperature co-electrolysis of H _(2) O and CO _(2) via the internal reverse water-gas shift (RWGS) reaction, may be meaningful. In this study, the influence of the H _(2) ?:?CO _(2) ratio on the activity, selectivity and stability of the as-prepared La _(0.75) Sr _(0.25) Cr _(0.5) Mn _(0.5) O _(3? δ ) (LSCrM) and Ni _(3) Sn _(2) as well as commercial Ni and Gd-doped CeO _(2) (GDC _(20) ) powder materials for the reverse RWGS reaction was investigated in a tubular quartz glass reactor at 700 °C and 800 °C and ambient pressure. The highest conversion factor close to the maximum value of 50% for CO was yielded for the LSCrM, Ni and GDC _(20) samples by applying a 0.5?:?0.5 H _(2) ?:?CO _(2) feed ratio at 800 °C. Similar activity was calculated for the Ni _(3) Sn _(2) alloy after normalization to the Ni mass content. Moreover, all the investigated catalysts exhibited higher selectivity for CO and H _(2) O products than Ni, with which CH _(4) molar concentrations up to 0.9% and 2.4% were collected at 800 °C and 700 °C, respectively. The influence of feed pressure on the carburisation process was inspected in a tubular Ni–Cr reactor. Under a carbon-rich gas mixture at 3 bar and 700 °C, large amounts of graphitic carbon were deposited solely on the Ni sample after 100 h of exposure time. After the exposure of the powder materials to 0.5?:?0.5 and 0.9?:?0.1 H _(2) ?:?CO _(2) atmospheres for 300 h at 700 °C and 10 bar, traces of amorphous carbon were surprisingly detected only on Ni _(3) Sn _(2) powder via Raman microscopy. Thus, because GDC _(20) ist not active for electrochemical H _(2) production, LSCrM or a mixture of both LSCrM and GDC _(20) materials appears to be the most promising candidate for Ni substitution in high-temperature H _(2) O/CO _(2) co-electrolysis.