Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-03-30 , DOI: 10.1016/j.apcatb.2020.118938 Zhao Sun , Tianyi Cai , Christopher K. Russell , J. Karl Johnson , Run-Ping Ye , Wenguo Xiang , Xiaoping Chen , Maohong Fan , Zhiqiang Sun
Catalytic methane decomposition (CMD) due to its various potentials including production of COx free H2 and technically simpleness, but is very challenging due to the lack of efficient, stable, and carbon-separable catalysts. An innovative chemical looping methane decomposition with CO2 reduction (CLMDCR) was developed to bridge the gap via the reduction → CMD → oxidation looping of a catalytic oxygen carrier (COC) for H2 production, deposited carbon separation, and CO2 reduction to CO. As high as 96.3 vol.% and 95.2 vol.% purities of H2 and CO can be generated using the COC (NiyFe3-yO4-Ca2FexAl2-xO5), superior to those obtained with state-of-the-art CH4 dry reforming. The COC shows not only high activities but also remarkable durability as demonstrated with 20 cyclic CLMDCR tests. Experimental results indicate that the long-term redox durability of COC is attributed to its atomic homogenization through the phase transformations of NiyFe3-yO4 ↔ Ni-Fe and Ca2Fe1.52Al0.48O5 ↔ CaO + Fe + Ca2FexAl2-xO5.
中文翻译:
通过Ca 2 Fe x Al 2-x O 5负载的Ni y Fe 3-y O 4纳米颗粒的氧化还原循环,将甲烷高效分解为H 2并将CO 2还原为CO
催化甲烷分解(CMD)由于其各种潜力,包括无CO x的H 2的产生和技术上的简单性,但由于缺乏有效,稳定且可与碳分离的催化剂而极富挑战性。开发了一种创新的具有CO 2还原的化学环甲烷分解(CLMDCR),通过还原→CMD→催化氧气载体(COC)的氧化环来弥合间隙,以生产H 2,沉积碳分离和将CO 2还原为CO 。使用COC(Ni y Fe 3-y O 4 -Ca 2可以产生96.3 vol。%和95.2 vol。%的纯度的H 2和COFe x Al 2-x O 5),优于采用最新的CH 4干重整法获得的那些。如20个循环CLMDCR测试所示,COC不仅显示出高活性,而且还具有出色的耐久性。实验结果表明,COC的长期氧化还原耐久性是通过镍的相转变归因于其原子均质ý的Fe 3-Y ø 4 ↔镍-铁和Ca 2的Fe 1.52铝0.48 ø 5 ↔的CaO +铁+钙2 Fe x Al 2-x O 5。