Designing an Electron-Deficient Pd/NiCo2O4 Bifunctional Electrocatalyst with an Enhanced Hydrodechlorination Activity to Reduce the Consumption of Pd,Environmental Science & Technology

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Designing an Electron-Deficient Pd/NiCo2O4 Bifunctional Electrocatalyst with an Enhanced Hydrodechlorination Activity to Reduce the Consumption of Pd
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-07-01 , DOI: 10.1021/acs.est.1c01922
Weiting Yu ₁ , He Jiang ₁ , Jinhui Fang ₁ , Shuang Song ₁

Affiliation

Reducing the Pd loading on electrodes is critical in the electrocatalytic hydrodechlorination (EHDC) of chlorinated organic compounds (COCs). The EHDC reaction of COCs on Pd involves three steps: H* formation, H* adsorption, and dechlorination. It has been established that the initial hydrogen evolution reaction (HER) occurs on Pd⁰ and the dechlorination steps occur on Pd²⁺. A strategy is proposed to design new electrodes by adding a reducible HER-active interlayer to replace Pd⁰, fulfilling the responsibility of producing hydrogen, and to facilitate the formation of more Pd²⁺ for following C–Cl bond cleavage. Keeping the atomic hydrogen adsorption energy on the Pd/interlayer similar to that on pure Pd is also necessary for H* adsorption as well as to maintain a high EHDC activity. For the first time, the NiCo₂O₄-interlayer-modified Pd/Ni-foam electrode was applied in the EHDC of COCs, which enhanced the EHDC efficiency to 100% within 90 min and reduced 88.6% of Pd consumption. The Pd/NiCo₂O₄/Ni-foam electrode with enhanced EHDC activity was also observed with almost 100% product selectivity and good stability. A synergistic mechanism is proposed for the enhanced EHDC activity on the Pd/NiCo₂O₄/Ni-foam. This work offers a simple and useful strategy to design robust electrocatalysts for the EHDC of COCs.

中文翻译：

设计一种具有增强加氢脱氯活性的缺电子 Pd/NiCo2O4 双功能电催化剂以减少 Pd 的消耗

减少电极上的 Pd 负载对于氯化有机化合物 (COC) 的电催化加氢脱氯 (EHDC) 至关重要。COCs 在 Pd 上的 EHDC 反应包括三个步骤：H* 形成、H* 吸附和脱氯。已经确定初始析氢反应 (HER) 发生在 Pd ^{0 上}，脱氯步骤发生在 Pd ^{2+ 上}。提出了一种设计新电极的策略，通过添加可还原的 HER 活性中间层来替代 Pd ⁰，履行产生氢的责任，并促进更多 Pd ²⁺的形成用于后续的 C-Cl 键断裂。保持 Pd/夹层上的原子氢吸附能与纯 Pd 上的原子氢吸附能相似也是 H* 吸附以及保持高 EHDC 活性所必需的。首次将NiCo ₂ O ₄夹层改性Pd/Ni泡沫电极应用于COCs的EHDC，在90分钟内将EHDC效率提高到100%，并降低了88.6%的Pd消耗。还观察到具有增强的 EHDC 活性的 Pd/NiCo ₂ O ₄ /Ni 泡沫电极具有几乎 100% 的产物选择性和良好的稳定性。提出了一种协同机制来增强 Pd/NiCo ₂ O ₄上的 EHDC 活性/镍泡沫。这项工作为设计用于 COC 的 EHDC 的强大电催化剂提供了一种简单而有用的策略。

更新日期：2021-07-20

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