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Reaction mechanism of N-(4-hydroxyphenyl)ethanamide electrodegradation via phosphorus-graphene prepared from triphenylphosphine: Generation and destruction of the reactive species
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-07-19 , DOI: 10.1016/j.cej.2020.126322
Yong-bo Yu , Qian Zhang , Li-ying Wu , Yu-lian Zhou , Bing-xin Wang , Bor-Yann Chen , Jun-ming Hong

Electrocatalysis as effective method for organic pollutants treatment, is greatly depended on the anode material. Graphene as wide used inorganic metal-free material could greatly improve by heteroatom doping. In this study, phosphorus-doped graphene (P-GN) was successfully prepared with triphenylphosphine as the phosphorus source and applied in the electrocatalytic oxidation of N-(4-hydroxyphenyl)ethanamide. The doping morphology of phosphorus was controlled by annealing temperature, and rising temperature could gradually alter the morphology of phosphorus from P-C to P-O. P-GN (20%–500 °C) had the best catalytic efficiency (91%) after 90 min of reaction, and the most active P species were confirmed as -CPO3, P-C, P-O, and -PO2 (from XPS). Those P species as catalyst could accelerate the generation of active chlorine for oxidation. However, the existence of O2 will weaken the seizing of electrons and increase the energy barrier of Cl- connection. The discussion of “P species regulate → P active species → active chlorine generation and destruction” could provide deep understanding of underlying mechanism.



中文翻译:

三苯基膦制备的磷-石墨烯电催化N-(4-羟苯基)乙酰胺电分解的反应机理:反应物种的产生和破坏

电催化作为处理有机污染物的有效方法,在很大程度上取决于阳极材料。石墨烯作为广泛使用的无机无金属材料,可以通过杂原子掺杂大大改善。本研究成功地以三苯基膦为磷源制备了掺磷石墨烯(P-GN),并将其应用于N-(4-羟苯基)乙酰胺的电催化氧化。磷的掺杂形态受退火温度的控制,温度的升高会逐渐改变磷的形态,从PC到PO。反应90分钟后,P-GN(20%–500°C)的催化效率最高(91%),并且活性最高的P种类被确认为-CPO 3,PC,PO和-PO 2(来自XPS)。那些作为催化剂的P物种可以促进氧化活性氯的生成。但是,O 2的存在会削弱电子的捕获并增加Cl连接的能垒。对“ P物种调控→P活性物种→活性氯的产生和破坏”的讨论可以提供对潜在机理的深刻理解。

更新日期:2020-07-23
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