A novel synergetic effect between Ru and Cu nanoparticles for Ru-Cu/Al2O3 causes highly efficient photothermocatalytic CO2 reduction with good durability
A novel synergetic effect between Ru and Cu nanoparticles for Ru-Cu/Al2O3 causes highly efficient photothermocatalytic CO2 reduction with good durability
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DOI：
10.1016/j.apsusc.2021.149821
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发表时间：
2021-04
影响因子：
6.7
通讯作者：
An Zhang;Shaowen Wu;Yuanzhi Li;Qian Zhang;Q. Hu;Jichun Wu;X. Tan;Yongdi Zhang
中科院分区：
文献类型：
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作者：
An Zhang;Shaowen Wu;Yuanzhi Li;Qian Zhang;Q. Hu;Jichun Wu;X. Tan;Yongdi Zhang
制备了不同Ru负载量的Al 2 O3共负载Ru和Cu纳米颗粒的纳米复合材料。Ru-Cu/Al 2 O3纳米复合材料很好地结合了Ru纳米颗粒的优异热催化活性和Cu纳米颗粒的高效光热转换，这是由于它们具有强的表面等离子体吸收。在500 W白炽灯聚焦照射下，它们对甲烷光催化还原CO2反应（CRM）表现出很高的催化活性。在聚焦的UV-vis-IR照明下，获得了非常高的H2（rH 2）和CO（rCO）的产生速率（59.24和63.91 mmol min−1g−1）和光燃料效率（η，33.1%）。即使在聚焦的λ > 560 nm可见-IR照明下，也获得了29.2%的非常高的η。由于碳沉积的副反应被阻断，纳米复合材料显示出非常好的光热催化耐久性，而负载在Al 2 O3上的Cu纳米颗粒（Cu/Al 2 O3）的参比催化剂由于Cu纳米颗粒上严重的碳沉积而迅速失去光热催化活性。发现Ru-Cu/Al 2 O3中Ru和Cu纳米颗粒之间的一种新的协同效应阻止了Cu纳米颗粒上严重的积碳，从而极大地提高了光热催化的耐久性。这归因于Cu纳米颗粒上的碳物种的氧化被Ru纳米颗粒迁移的氧物种（由CO2解离形成）加速。一种新的光活化被发现，大大促进光驱动的热催化CRM上Ru-Cu/Al 2 O3由于表观活化能被大大降低后，聚焦照明。这与Ru-Cu/Al_2 O_3上CRM的氧物种氧化碳物种的速率决定步骤有关。
Nanocomposites of Ru and Cu nanoparticles co-supported on Al2O3with different Ru loadings were prepared. The Ru-Cu/Al2O3nanocomposites well integrates excellent thermocatalytic activity of Ru nanoparticles with efficient photothermal conversion of Cu nanoparticles due to their strong surface plasmonic absorption. They show very high catalytic activity for photothermocatalytic CO2reduction by methane (CRM) under focused illumination from a 500 W Xe lamp. Very high production rates of H2(rH2) and CO (rCO) (59.24 and 63.91 mmol min−1g−1) and light-to-fuel efficiency (η, 33.1%) are acquired under focused UV–vis-IR illumination. Even under focused λ > 560 nm vis-IR illumination, a very highηof 29.2% is acquired. The nanocomposites show very good photothermocatalytic durability due to the side-reactions of carbon deposition being blocked, while a reference catalyst of Cu nanoparticles supported on Al2O3(Cu/Al2O3) quickly loses photothermocatalytic activity due to severe carbon deposition on Cu nanoparticles. A novel synergetic effect between Ru and Cu nanoparticles for Ru-Cu/Al2O3is found to block the severe carbon deposition on Cu nanoparticles, thus tremendously promoting photothermocatalytic durability. This is ascribed to the oxidation of carbon species on Cu nanoparticles being accelerated by oxygen species (formed by CO2dissociation) migrated from Ru nanoparticles. A novel photoactivation is found to substantially promote light-driven thermocatalytic CRM on Ru-Cu/Al2O3due to the apparent activation energy being immensely reduced upon the focused illumination. This is associated with the rate determining step of the oxidation of carbon species by oxygen species for CRM on Ru-Cu/Al2O3being accelerated upon the focused illumination.