CO2 Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments,ACS Energy Letters

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CO2 Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-08-15 , DOI: 10.1021/acsenergylett.4c01866
Kyra M. K. Yap _{1,

2,

3} , Aisulu Aitbekova _{3,

4} , Matthew Salazar _{3,

5} , Tobias A. Kistler _{3,

6} , Melanie Rodríguez Pabón _{2,

3} , Magel P. Su _{3,

4} , Nicholas B. Watkins _{3,

5} , Sang-Won Lee _{1,

2,

3} , Peter Agbo _{3,

6} , Adam Z. Weber _{3,

6} , Jonas C. Peters _{3,

5} , Theodor Agapie _{3,

5} , Adam C. Nielander _{1,

3} , Harry A. Atwater _{3,

4} , Thomas F. Jaramillo _{1,

2,

3} , Alexis T. Bell _{3,

6,

7}

Affiliation

We developed a tandem, unassisted, solar-driven electrochemical and photothermocatalytic process for the single-pass conversion of CO₂ to butene using only simulated solar irradiation as the energetic input. The two-step process involves electrochemical CO₂ reduction (CO₂R) to ethylene followed by ethylene dimerization to butene. We assessed two unassisted electrochemical setups to concentrate ethylene in the CO₂R reactor, achieving concentrations up to 5.4 vol% with 1.8% average solar-to-ethylene conversion and 5.6% average CO₂-to-ethylene single-pass conversion under 1-sun illumination. When the effluent electrochemical gas stream was passed through the photothermocatalytic ethylene oligomerization reactor, we generated 600 ppm of butene under 3-sun illumination. Through analysis of this process, we identified that the presence of H₂, CO, and H₂O leads to rapid deactivation of the Ni-based ethylene oligomerization catalyst.

中文翻译：

通过串联光伏-电化学/光热催化过程将二氧化碳转化为丁烯：耦合微环境的协同设计方法

我们开发了一种串联、无辅助、太阳能驱动的电化学和光热催化工艺，仅使用模拟太阳辐射作为能量输入，将 CO ₂单程转化为丁烯。该两步法涉及电化学CO ₂还原(CO ₂ R)为乙烯，随后乙烯二聚为丁烯。我们评估了两种在 CO ₂ R 反应器中浓缩乙烯的无辅助电化学装置，在 1- 条件下实现了高达 5.4 vol% 的浓度，平均太阳能转化为乙烯的转化率为 1.8%，CO ₂转化为乙烯的平均单程转化率为 5.6%太阳照明。当流出的电化学气流通过光热催化乙烯低聚反应器时，我们在 3 太阳光照下产生了 600 ppm 的丁烯。通过对该过程的分析，我们发现H ₂ 、CO和H ₂ O的存在会导致镍基乙烯齐聚催化剂快速失活。

更新日期：2024-08-15

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