Sorption-enhanced reforming and gasification (SERG) offers a promising approach to intensify hydrogen production from carbonaceous feedstocks. However, conventional sorbents require substantial temperature increases for the endothermic CO2 release step and are prone to deactivation. This study introduces a new class of redox-activated sorbents capable of stable isothermal operation and tunable heats of reactions, thereby facilitating an efficient reactive separation scheme. Using plane-wave density functional theory (DFT) calculations of structures and free energies, we screened 1225 perovskite-structured sorbent candidates, followed with extensive experimental validation. An effective descriptor, (ΔGabs + ΔGreg), was identified to expedite sorbent optimization. The advanced sorbents showed reversible, isothermal carbonation of up to 78% of the A-site cation, permitting isothermal SERG or "iSERG". Their versatility was demonstrated in a fluidized bed for woody biomass gasification and a packed bed for biogas conversion, yielding hydrogen-enriched (76 vol.%) syngas from biomass and 95+% pure H2 from biogas. Our results also support integrated CO2 capture to produce carbon-negative hydrogen products.

中文翻译：

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复杂氧化物的高通量设计作为等温、氧化还原激活的二氧化碳吸附剂用于绿色制氢


吸附强化重整和气化（SERG）提供了一种有前途的方法来强化碳质原料的氢气生产。然而，传统吸附剂在吸热二氧化碳释放步骤中需要大幅提高温度，并且容易失活。这项研究引入了一类新型氧化还原激活吸附剂，能够稳定等温操作和可调反应热，从而促进有效的反应分离方案。利用平面波密度泛函理论 (DFT) 计算结构和自由能，我们筛选了 1225 种钙钛矿结构候选吸附剂，随后进行了广泛的实验验证。确定了一个有效的描述符（ΔGabs + ΔGreg）来加速吸附剂优化。先进的吸附剂显示出高达 78% 的 A 位阳离子的可逆等温碳酸化，从而允许等温 SERG 或“iSERG”。它们的多功能性在用于木质生物质气化的流化床和用于沼气转化的填充床中得到了证明，从生物质中产生富氢（76体积％）的合成气，并从沼气中产生95％以上的纯氢气。我们的结果还支持综合二氧化碳捕获来生产碳负氢产品。