Suppressing product crossover and C–C bond cleavage in a glycerol membrane electrode assembly reformer,Energy & Environmental Science

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Suppressing product crossover and C–C bond cleavage in a glycerol membrane electrode assembly reformer
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2024-08-01 , DOI: 10.1039/d4ee01824a
Chencheng Dai _{1,

2} , Qian Wu ₁ , Tianze Wu ₁ , Yuwei Zhang ₁ , Libo Sun _{2,

3,

4} , Xin Wang _{3,

4} , Adrian C. Fisher _{2,

5} , Zhichuan J. Xu _{1,

2,

6,

7}

Affiliation

Generating hydrogen through water electrolysis is impeded by high costs and substantial energy consumption mainly due to high equilibrium potential and sluggish kinetics of the oxygen evolution reaction (OER). Glycerol oxidation reaction (GOR) is proposed as an alternative due to its low thermodynamic limit and value-added oxidation products. However, GOR in membrane electrolyzers faces challenges in achieving industrial-scale current densities as well as in addressing crossover issues. Here, we investigated five different membrane electrode assembly (MEA) configurations to perform GOR with various ion exchange membranes and catholyte. After systematic study, we present an innovative acid–alkali asymmetric cell design which operates with alkaline anolyte and acidic catholyte for electrochemical neutralization energy (ENE) harvesting to improve energy efficiency. The product anions crossover via anion exchange membrane (AEM) is also impeded since that the increasing concentration gradient-driven hydroxide ion crossover occupying the anion exchange channels in AEM and thus limits the product crossover of AEM. Such device also demonstrates the capability of impeding C–C bond cleavage to promote high-value C3 products generation and reduce carbon emission due to the lower degree of cell polarization and limited hydroxide ion supply at anode. Eventually, a whole-cell potential can be significantly reduced to 0.377 V while achieving a current density of 200 mA cm⁻². Moreover, total faradaic efficiencies (FEs) of 55% and 84% for all C3 products and all liquid products can be achieved at a current density up to 1000 mA cm⁻².

中文翻译：

抑制甘油膜电极组件重整器中的产物交叉和 C-C 键断裂

通过水电解制氢受到高成本和大量能源消耗的阻碍，这主要是由于高平衡电位和析氧反应（OER）动力学缓慢。甘油氧化反应（GOR）因其热力学极限低和氧化产物增值而被提议作为替代反应。然而，膜电解槽中的 GOR 在实现工业规模电流密度以及解决交叉问题方面面临挑战。在这里，我们研究了五种不同的膜电极组件 (MEA) 配置，以使用各种离子交换膜和阴极电解液执行 GOR。经过系统研究，我们提出了一种创新的酸碱不对称电池设计，它使用碱性阳极电解液和酸性阴极电解液进行电化学中和能量（ENE）收集，以提高能源效率。通过阴离子交换膜（AEM）的产物阴离子交叉也受到阻碍，因为增加的浓度梯度驱动的氢氧根离子交叉占据了AEM中的阴离子交换通道，从而限制了AEM的产物交叉。由于电池极化程度较低和阳极氢氧离子供应有限，该装置还具有阻止 C-C 键断裂的能力，可促进高价值 C3 产品的生成并减少碳排放。最终，全细胞电位可以显着降低至0.377 V，同时实现200 mA cm ^-2的电流密度。此外，所有C3产品和所有液体产品的总法拉第效率（FE）可以在高达1000 mA cm ^-2的电流密度下实现55%和84%。

更新日期：2024-08-06

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