Bio-Electrocatalytic Conversion of Food Waste to Ethylene via Succinic Acid as the Central Intermediate.
Bio-Electrocatalytic Conversion of Food Waste to Ethylene via Succinic Acid as the Central Intermediate.
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DOI：
10.1021/acscatal.2c02689
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发表时间：
2022-11-04
期刊：
影响因子：
12.9
通讯作者：
Reisner, Erwin
中科院分区：
文献类型：
--
作者：
Pichler, Christian M.;Bhattacharjee, Subhajit;Lam, Erwin;Su, Lin;Collauto, Alberto;Roessler, Maxie M.;Cobb, Samuel J.;Badiani, Vivek M.;Rahaman, Motiar;Reisner, Erwin
关键词：
乙烯是化学工业中的重要原料，但目前需要从化石资源生产。琥珀酸的电催化氧化脱羧提供了原则上环境友好的路线来产生乙烯。在这里，不同的碳电极材料和特性的作用的详细调查表明，平坦的电极表面和高有序的碳材料是有利于反应。一系列电化学和光谱学方法，如Koutecky-Levich分析，旋转环盘电极（RRDE）研究和塔菲尔分析以及量子化学计算，电子顺磁共振（EPR）和原位红外（IR）光谱产生了对整个过程机制的进一步见解。检测到不同的反应中间体，并且确定脱羧起始电位相对于可逆氢电极（RHE）为2.2- 2.3V。在机理研究和电极优化的基础上，建立了一种利用餐厨垃圾中的琥珀酸生产乙烯的两步生物电化学过程。该集成方法的初始步骤涉及食品废物的微生物水解/发酵成含有琥珀酸的水溶液（0.3 M; 3.75 mmol/g烘焙废物）。第二步是在室温下用流动装置将得到的中间体丁二酸电氧化为乙烯，产率为0.4-1 μmol乙烯cm电极-2 h-1。这种方法提供了一种替代策略，在环境条件下使用可再生能源从食物垃圾中生产乙烯。
Ethylene is an important feedstock in the chemical industry, but currently requires production from fossil resources. The electrocatalytic oxidative decarboxylation of succinic acid offers in principle an environmentally friendly route to generate ethylene. Here, a detailed investigation of the role of different carbon electrode materials and characteristics revealed that a flat electrode surface and high ordering of the carbon material are conducive for the reaction. A range of electrochemical and spectroscopic approaches such as Koutecky–Levich analysis, rotating ring-disk electrode (RRDE) studies, and Tafel analysis as well as quantum chemical calculations, electron paramagnetic resonance (EPR), and in situ infrared (IR) spectroscopy generated further insights into the mechanism of the overall process. A distinct reaction intermediate was detected, and the decarboxylation onset potential was determined to be 2.2–2.3 V versus the reversible hydrogen electrode (RHE). Following the mechanistic studies and electrode optimization, a two-step bio-electrochemical process was established for ethylene production using succinic acid sourced from food waste. The initial step of this integrated process involves microbial hydrolysis/fermentation of food waste into aqueous solutions containing succinic acid (0.3 M; 3.75 mmol per g bakery waste). The second step is the electro-oxidation of the obtained intermediate succinic acid to ethylene using a flow setup at room temperature, with a productivity of 0.4–1 μmol ethylene cmelectrode–2 h–1. This approach provides an alternative strategy to produce ethylene from food waste under ambient conditions using renewable energy.
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影响因子：
56.9
作者：
Dinh, Cao-Thang;Burdyny, Thomas;Sargent, Edward H.
通讯作者：
Sargent, Edward H.
影响因子：
10.4
作者：
Castellani, Beatrice;Rinaldi, Sara;Rossi, Federico
通讯作者：
Rossi, Federico
DOI：
10.1016/j.checat.2022.02.014
发表时间：
2022-05-19
期刊：
CHEM CATALYSIS
影响因子：
--
作者：
Liu, Sihang;Govindarajan, Nitish;Chan, Karen
通讯作者：
Chan, Karen
影响因子：
3.9
作者：
LEVY, PF;SANDERSON, JE;CHENG, LK
通讯作者：
CHENG, LK
影响因子：
56.9
作者：
Liu, Chong;Colon, Brendan C.;Nocera, Daniel G.
通讯作者：
Nocera, Daniel G.