Polystyrene Waste Thermochemical Hydrogenation to Ethylbenzene by a N-Bridged Co, Ni Dual-Atom Catalyst,Journal of the American Chemical Society

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Polystyrene Waste Thermochemical Hydrogenation to Ethylbenzene by a N-Bridged Co, Ni Dual-Atom Catalyst
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-07-12 , DOI: 10.1021/jacs.3c05184
Runze Li ₁ , Zedong Zhang ₁ , Xiao Liang ₁ , Ji Shen ₁ , Jia Wang _{2,

3} , Wenming Sun ₄ , Dingsheng Wang ₁ , Jianchun Jiang _{2,

3} , Yadong Li _{1,

5}

Affiliation

Recycling waste plastics requires the degradation of plastics into small molecules. However, various products are widely distributed using traditional methods of depolymerizing polystyrene (PS) such as catalytic pyrolysis and hydrogenolysis. Here, we creatively report a N-bridged Co, Ni dual-atom (Co-N-Ni) catalyst for the targeted conversion of waste PS plastics to ethylbenzene via a pressurized tandem fixed-bed reactor where hydropyrolysis is coupled with downstream vapor-phase hydrotreatment. The Co-N-Ni catalyst achieves 95 wt % PS conversion with 92 wt % ethylbenzene yield, significantly superior to the corresponding single-atom catalysts, and enables degradation of real PS plastics. Theoretical calculations and experimental results demonstrate that the d-band center of metal atoms is well regulated in the Co-N-Ni catalyst. The Co site activates the C═C bond more easily, while the Ni site spatially optimizes the adsorption configuration of the styrene molecule due to the electronic interaction. This Co-N-Ni catalyst in the tandem reactor also shows excellent durability and provides a new direction for real plastic degradation.

中文翻译：

N桥Co、Ni双原子催化剂聚苯乙烯废料热化学加氢制乙苯

回收废塑料需要将塑料降解成小分子。然而，使用催化热解和氢解等传统解聚聚苯乙烯（PS）方法广泛分布的各种产品。在这里，我们创造性地报道了一种N桥联Co、Ni双原子（Co-N-Ni）催化剂，通过加压串联固定床反应器将废PS塑料定向转化为乙苯，其中加氢热解与下游气相耦合加氢处理。Co-N-Ni催化剂实现了95 wt%的PS转化率和92 wt%的乙苯收率，明显优于相应的单原子催化剂，并且能够降解真正的PS塑料。理论计算和实验结果表明，Co-N-Ni催化剂中金属原子的d带中心得到了很好的调控。Co位点更容易激活C=C键，而Ni位点由于电子相互作用而在空间上优化了苯乙烯分子的吸附构型。这种串联反应器中的Co-N-Ni催化剂还表现出优异的耐久性，为真正的塑料降解提供了新的方向。

更新日期：2023-07-12

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