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Efficient Electrochemical‐Enzymatic Conversion of PET to Formate Coupled with Nitrate Reduction over Ru‐Doped Co3O4 Catalysts
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2025-03-19 , DOI: 10.1002/anie.202421240
Jiadi Jiang 1 , Leting Zhang 2 , Guanzheng Wu 3 , Jianrui Zhang 4 , Yidong Yang 3 , Wenhui He 5 , Jun Zhu 6 , Jian Zhang 7 , Qing Qin 8
Affiliation  

Electrochemical reforming presents a sustainable route for the conversion of nitrate (NO3‐) and polyethylene terephthalate (PET) into value‐added chemicals, such as ammonia (NH3) and formic acid (HCOOH). However, its widespread application has been constrained by low selectivity due to the complexity of reduction processes and thus energy scaling limitations. In this study, the atomically dispersed Ru sites in Co3O4 synergistically interact with Co centers, facilitating the adsorption and activation of hydroxyl radicals (OH*) and ethylene glycol (EG), resulting in a remarkable HCOOH selectivity of 99 % and a yield rate of 11.2 mmol h‐1 cm‐2 surpassing that of pristine Co3O4 (55 % and 3.8 mmol h‐1 cm‐2). Furthermore, when applied as a bifunctional cathode catalyst, Ru‐Co3O4 achieves a remarkable Faradaic efficiency (FE) of 98.5 % for NH3 production (3.54 mmol h‐1 cm‐2) at ‐0.3 V vs. RHE. Additionally, we developed a prototype device powered by a commercial silicon photovoltaic cell, enabling on‐site solar‐driven production of formate and NH3 through enzyme‐catalyzed PET and NO3‐ conversion. This study offers a viable approach for waste valorization and green chemical production, paving the way for sustainable energy applications.

中文翻译:


通过 Ru 掺杂 Co3O4 催化剂实现 PET 向甲酸盐的高效电化学酶促转化与硝酸盐还原



电化学重整为将硝酸盐 (NO3‐) 和聚对苯二甲酸乙二醇酯 (PET) 转化为增值化学品提供了一种可持续的途径,例如氨 (NH3) 和甲酸 (HCOOH)。然而,由于还原过程的复杂性和能量缩放的限制,其广泛应用受到低选择性的限制。在本研究中,Co3O4 中原子分散的 Ru 位点与 Co 中心协同相互作用,促进羟基自由基 (OH*) 和乙二醇 (EG) 的吸附和激活,从而产生 99% 的显着 HCOOH 选择性和 11.2 mmol h-1 cm-2 的产率,超过了原始 Co3O4 (55% 和 3.8 mmol h-1 cm-2)。此外,当用作双功能阴极催化剂时,Ru-Co3O4 在 -0.3 V 下与 RHE 相比,在 -0.3 V 下实现了 98.5% 的 NH3 生产法拉第效率 (FE)(3.54 mmol h-1 cm-2)。此外,我们还开发了一种由商用硅光伏电池供电的原型设备,通过酶催化的 PET 和 NO3 转化实现现场太阳能驱动的甲酸盐和 NH3 生产。这项研究为废物增值和绿色化学品生产提供了一种可行的方法,为可持续能源应用铺平了道路。
更新日期:2025-03-19
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