Abstract In order to explore the efficient and clean technology for methanol production from shale gas, this work firstly presents shale gas chemical looping reforming processes for methanol and hydrogen co-production using three types of fuels (purge gas, shale gas and purge gas, and hydrogen and purge gas), which are directly combusted by air for heating the reforming reactors. In these processes, the important parameters of oxygen carrier flow, steam flow, air flow, and recycle ratio of unreacted syngas have been optimized to maximize methanol and hydrogen production and energy saving. The novel processes with hydrogen and purge gas as fuel have low exergy efficiencies between 74.6% and 75.1%. The process with shale gas as fuel has high exergy efficiency of 76.7% with productions of methanol-2158 kmol/h and hydrogen-937 kmol/h, while it possesses the highest CO2 emissions of 580 kmol/h. This work further integrates chemical looping reforming and combustion to reduce the CO2 emissions. The chemical looping combustion technology makes its direct CO2 emissions as low as about 39 kmol/h, significantly lower than the first three processes. The exergy efficiencies of the last process without and with considering the CO2 exergy as product exergy can be reached at as high as 76.8% and 77.5%, respectively. Obviously, the integration between chemical looping reforming and combustion has obvious competitive advantages and application prospect for efficient and green production of methanol and hydrogen.

中文翻译：

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高效清洁生产甲醇和氢气的页岩气化学回路重整工艺系统优化及性能评价

摘要 为探索高效、清洁的页岩气制甲醇技术，本工作首先介绍了利用三种燃料（吹扫气、页岩气和吹扫气）进行甲醇和氢气联产的页岩气化学回路重整工艺，以及氢气和吹扫气），它们被空气直接燃烧以加热重整反应器。在这些工艺中，氧载体流量、蒸汽流量、空气流量和未反应合成气的回收率等重要参数都得到了优化，以最大限度地提高甲醇和氢气的产量和节能效果。以氢气和吹扫气体为燃料的新工艺的火用效率低，介于 74.6% 和 75.1% 之间。以页岩气为燃料的工艺火用效率高达76.7%，甲醇产量为2158 kmol/h，氢气产量为937 kmol/h，而它的二氧化碳排放量最高，达到 580 kmol/h。这项工作进一步整合了化学循环重整和燃烧，以减少二氧化碳排放。化学循环燃烧技术使其直接二氧化碳排放量低至约 39 kmol/h，明显低于前三种工艺。不考虑和考虑 CO2 火用作为产品火用的最后一个过程的火用效率可分别高达 76.8% 和 77.5%。显然，化学链重整与燃烧相结合，在高效绿色生产甲醇和氢气方面具有明显的竞争优势和应用前景。化学循环燃烧技术使其直接二氧化碳排放量低至约 39 kmol/h，明显低于前三种工艺。不考虑和考虑 CO2 火用作为产品火用的最后一个过程的火用效率可分别高达 76.8% 和 77.5%。显然，化学链重整与燃烧相结合，在高效绿色生产甲醇和氢气方面具有明显的竞争优势和应用前景。化学循环燃烧技术使其直接二氧化碳排放量低至约 39 kmol/h，明显低于前三种工艺。不考虑和考虑 CO2 火用作为产品火用的最后一个过程的火用效率可分别高达 76.8% 和 77.5%。显然，化学链重整与燃烧相结合，在高效绿色生产甲醇和氢气方面具有明显的竞争优势和应用前景。