Heterojunction-redox catalysts of FexCoyMg10CaO for high-temperature CO2 capture and in situ conversion in the context of green manufacturing,Energy & Environmental Science

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Heterojunction-redox catalysts of FexCoyMg10CaO for high-temperature CO2 capture and in situ conversion in the context of green manufacturing
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-12-18 , DOI: 10.1039/d0ee03320k
Bin Shao _{1,

2,

3,

4} , Guihua Hu _{2,

3,

4,

5} , Khalil A. M. Alkebsi _{2,

3,

4,

5} , Guanghua Ye _{2,

3,

4,

6} , Xiaoqing Lin _{1,

2,

3,

4} , Wenli Du _{2,

3,

4,

5} , Jun Hu _{1,

2,

3,

4} , Meihong Wang _{7,

8,

9,

10} , Honglai Liu _{1,

2,

3,

4} , Feng Qian _{2,

3,

4,

5}

Affiliation

The integration of carbon capture and CO₂ utilization could be a promising solution to the crisis of global warming. By integrating calcium-looping (CaL) and the reverse-water-gas-shift (RWGS) reaction, a high-temperature CO₂ capture and in situ conversion technology is successfully realized in one fixed-bed column at the same operating temperature of 650 °C. Inspired by the heterojunction photocatalytic mechanism, the heterojunction-redox catalysis strategy is proposed for the first time by doping the bimetallic Fe³⁺/Fe²⁺ and Co³⁺/Co²⁺ redox couples into a hierarchical porous CaO/MgO composite. The presence of different valence states of doped Fe and Co oxides not only provides extra oxygen vacancies to facilitate CO₂ adsorption, and hence adsorption enhanced conversion (AEC), but also significantly lowers the electric potential difference of Fe³⁺/Fe²⁺ through the newly formed Fermi level in Fe₅Co₅Mg₁₀CaO, which makes electron spillover easier to improve the catalytic activity in the RWGS reaction for CO₂ conversion. More importantly, with the high-temperature refractory MgO and the highly disperse Fe and Co oxides in Fe₅Co₅Mg₁₀CaO, the problem of CaO sintering is successfully solved. An excellent and stable high-temperature CO₂ capture capacity of 9.0–9.2 mmol g⁻¹, an in situ CO₂ conversion effeciency near 90% and a CO selectivity close to 100% are achieved in the integrated CaL/RWGS process. In addition, experimental and simulation scale-up studies further demonstrate its pratical scalability. Economic evaluation reveals that the integrated CaL/RWGS technology is much more cost-effective than the individual CaL and RWGS processes. Therefore, the heterojunction-redox strategy provides a unique way to design bifunctional adsorbent/catalyst materials. The integrated CaL/RWGS process could be a promising technology for CO₂ capture and utilization.

中文翻译：

FexCoyMg10CaO的异质结-氧化还原催化剂用于绿色制造中的高温CO2捕集和原位转化

碳捕获和CO ₂利用的整合可能是解决全球变暖危机的有前途的解决方案。通过整合钙环化（CaL）和逆水煤气变换（RWGS）反应，在同一工作温度为650的固定床色谱柱中成功实现了高温CO ₂捕获和原位转化技术℃。受异质结光催化机理的启发，通过掺杂双金属Fe ³⁺ / Fe ²⁺和Co ³⁺ / Co ²⁺首次提出异质结-氧化还原催化策略。氧化还原偶合成分层的多孔CaO / MgO复合材料。掺杂Fe和Co的氧化物的不同价态的存在不仅提供额外的氧空位，以促进CO ₂吸附，因此吸附增强变换（AEC），而且还降低了显著Fe的电势差³⁺ / Fe的²⁺通过Fe ₅ Co ₅ Mg ₁₀ CaO中新形成的费米能级使电子外溢更容易提高RWGS反应中CO ₂转化的催化活性。更重要的是，在Fe ₅ Co中使用高温耐火材料MgO和高度分散的Fe和Co氧化物₅ Mg₁₀ CaO，成功解决了CaO烧结问题。优异的和稳定的高温CO₂的捕获9.0-9.2容量mmol克^-1，一个原位CO₂在集成的CaL / RWGS工艺中，转化效率接近90％，CO选择性接近100％。此外，实验和仿真放大研究进一步证明了其实用的可扩展性。经济评估表明，集成的CaL / RWGS技术比单独的CaL和RWGS工艺更具成本效益。因此，异质结氧化还原策略提供了一种设计双功能吸附剂/催化剂材料的独特方法。集成的CaL / RWGS工艺可能是有前途的CO ₂捕集和利用技术。

更新日期：2021-01-13

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