当前位置: X-MOL 学术Nat. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide
Nature Catalysis ( IF 37.8 ) Pub Date : 2020-01-06 , DOI: 10.1038/s41929-019-0402-8
Chuan Xia , Seoin Back , Stefan Ringe , Kun Jiang , Fanhong Chen , Xiaoming Sun , Samira Siahrostami , Karen Chan , Haotian Wang

Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in situ produced O2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by sixfold to 66% with an overpotential of 640 mV, under which a H2O2 production rate of 23.4 µmol min−1 cm−2 (75.2 mA cm−2 partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.



中文翻译:

局限的局部氧气促进电化学水氧化成过氧化氢

电化学双电子水氧化法是替代蒽醌方法的一种可再生和现场生成H 2 O 2的有前途的途径。然而,由于与传统的四电子氧释放反应的激烈竞争,以及由于过大的电势和低的生产率,目前由于选择性低而受到限制。在这里,我们报告了一种界面工程方法,该方法通过用疏水性聚合物涂覆催化剂来限制原位产生的O 2气体,以调节水的氧化反应路径。使用碳催化剂作为模型系统,我们显示出固有的H 2 O-to-H 2 O 2显着增加与原始催化剂相比具有更高的选择性和活性。在640 mV的超电势下,最大H 2 O 2法拉第效率提高了六倍,达到66%,在这种情况下,H 2 O 2的生产率为23.4 µmol min -1 cm -2(75.2 mA cm -2分电流)。实现。这种方法已成功地扩展到镍金属,证明了我们当地的气体限制概念的广泛适用性。

更新日期:2020-01-06
down
wechat
bug