局部表面等离子共振增强连续流光电催化 CO2 转化为 CO,Energy & Fuels

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局部表面等离子共振增强连续流光电催化 CO2 转化为 CO
Energy & Fuels ( IF 5.2 ) Pub Date : 2022-06-23 , DOI: 10.1021/acs.energyfuels.2c01520
Xinze Bi ₁ , Hongzhi Wang ₁ , Zhongzue Yang ₁ , Yuezhu Zhao ₁ , Zhengguang Ma ₁ , Tengfei Liu ₁ , Mingbo Wu ₁

Affiliation

二氧化碳(CO ₂ )的光电催化(PEC)还原可以结合光催化和电催化的优点，在温和的条件下将CO ₂还原成高附加值的化工产品。然而，由于传质过程有限以及活性位点周围复杂的电场环境，催化剂的活性和产物的选择性仍不能令人满意。在这项工作中，PEC CO ₂转化为 CO 是通过等离子体 Au NR 在新的连续流动池反应器中有效实现的。得益于快速的传质过程和Au NRs 表面的高 CO _{2浓度，连续流通池反应器中的光电流密度约为 1.0 mA cm}^–2，约为传统 H 电池反应器 (0.17 mA cm ^–2 ) 的 5 倍。此外，由于 Au NR 的 LSPR 效应，CO 的法拉第效率在光照下增加了约 20%。DFT计算还用于比较CO ₂和CO在Au NRs表面的吸附能，解释了Au NRs在新型流通池反应器中具有更高活性和选择性的原因。综上所述，该工作为光电催化反应器提供了新的选择，为光电催化CO ₂还原的未来产业化奠定了基础。

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Localized Surface Plasmon Resonance Enhanced Continuous Flow Photoelectrocatalytic CO2 Conversion to CO

Photoelectrocatalytic (PEC) reduction of carbon dioxide (CO₂) could combine the advantages of photocatalysis and electrocatalysis and reduce CO₂ into high value-added chemical products in mild conditions. However, the activities of catalysts and selectivities of products are still not satisfactory because of the limited mass transfer progress and the complex electric field environment around active sites. In the work, PEC CO₂ conversion to CO is realized efficiently by plasmonic Au NRs in a new continuous flow cell reactor. Benefiting from the rapid mass transfer process and the high concentration of CO₂ on the Au NRs surface, the photocurrent density in the continuous flow cell reactor is about 1.0 mA cm^–2, which is about 5 times that in the traditional H-cell reactor (0.17 mA cm^–2). Besides, the Faraday efficiency of CO increased about 20% under light illumination resulting from the LSPR effect of Au NRs. The DFT calculation is also used to compare the adsorption energies of CO₂ and CO on the surfaces of Au NRs, explaining the reasons for the higher activities and selectivities of Au NRs in a new flow-cell reactor. In summary, this work provides a new choice for a photoelectrocatalytic reactor and lays the foundation for the future industrialization of photoelectrocatalytic CO₂ reduction.

更新日期：2022-06-23

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