Sustainable catalytic oxidation of 1,3-butadiene over dispersedly assembled Ce0.027W0.02Mn0.054TiOx featuring synergistic redox cycles,Environmental Science: Nano

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Sustainable catalytic oxidation of 1,3-butadiene over dispersedly assembled Ce0.027W0.02Mn0.054TiOx featuring synergistic redox cycles
Environmental Science: Nano ( IF 5.8 ) Pub Date : 2022-08-26 , DOI: 10.1039/d2en00414c
Qianqian Li _{1,

2} , Chuanqi Li _{1,

2} , Mengjing Wang ₃ , Guijin Su _{1,

2} , Bohua Sun _{1,

2} , Mingge Wu _{1,

2} , Zhiwei Zhou _{1,

2} , Jiaxin Pang _{1,

2} , Jing Meng _{1,

2} , Bin Shi _{1,

2}

Affiliation

The challenge of the difficult recovery of ubiquitous low-boiling point alkenes in industrial exhaust gas gives catalytic oxidation a vital role, which crucially needs developing cost-effective catalysts. Herein, seven Ti-based catalysts with varied introduction of trace W, Ce and Mn were fabricated and assembled for the oxidation of 1,3-butadiene at 150–300 °C. Ce_0.027W_0.02Mn_0.054TiO_x featuring multiple cations exhibited exceptional oxidation activity. Based on comprehensive experiments and crystal cell theoretical analysis, the excellent catalytic activity was majorly governed by remarkably synergistic redox cycles among components: Mn³⁺ + Ti⁴⁺ ↔ Mn⁴⁺ + Ti³⁺, W⁶⁺ + Ti³⁺ ↔ W⁵⁺ + Ti⁴⁺, W⁶⁺ + Mn³⁺ ↔ W⁵⁺ + Mn⁴⁺, W⁵⁺ + Ce⁴⁺ ↔ W⁶⁺ + Ce³⁺, and Ce³⁺ + Mn⁴⁺ ↔ Ce⁴⁺ + Mn³⁺. The electron transfer between the catalyst interior and interface endowed Ce_0.027W_0.02Mn_0.054TiO_x rich active oxygen species with a sustainable 100% CO₂ yield and certain anti-water interference. By combining the in situ dynamic oxidation process of 1,3-butadiene, a catalytic oxidation mechanism driven by synergistic redox cycles was proposed. The design of a multiple-cation catalyst featuring robust synergistic interactions could provide a new insight into the control of typical light alkenes.

中文翻译：

1,3-丁二烯在分散组装的 Ce0.027W0.02Mn0.054TiOx 上的可持续催化氧化，具有协同氧化还原循环

工业废气中普遍存在的低沸点烯烃难以回收的挑战使催化氧化发挥了至关重要的作用，这迫切需要开发具有成本效益的催化剂。在此，制备并组装了七种不同引入痕量 W、Ce 和 Mn 的 Ti 基催化剂，用于在 150-300°C 下氧化 1,3-丁二烯。Ce _0.027 W _0.02 Mn _0.054 TiO _x具有多种阳离子，表现出优异的氧化活性。基于综合实验和晶胞理论分析，优异的催化活性主要受组分之间显着协同的氧化还原循环控制：Mn ³⁺ + Ti ⁴⁺ ↔ Mn ⁴⁺+ Ti ³⁺ , W ⁶⁺ + Ti ³⁺ ↔ W ⁵⁺ + Ti ⁴⁺ , W ⁶⁺ + Mn ³⁺ ↔ W ⁵⁺ + Mn ⁴⁺ , W ⁵⁺ + Ce ⁴⁺ ↔ W ⁶⁺ + Ce ³⁺和 Ce ³⁺ + Mn ⁴⁺ ↔ Ce ⁴⁺ + Mn ³⁺。催化剂内部和界面之间的电子转移赋予了富含 Ce _0.027 W _0.02 Mn _0.054 TiO _x的活性氧物质和可持续的 100% CO ₂产量和一定的抗水干扰。通过结合1,3-丁二烯的原位动态氧化过程，提出了协同氧化还原循环驱动的催化氧化机制。具有强大协同作用的多阳离子催化剂的设计可以为控制典型轻烯烃提供新的见解。

更新日期：2022-08-26

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