Academic Journal

pH effects on the electrochemical reduction of CO (2) towards C 2 products on stepped copper

التفاصيل البيبلوغرافية
العنوان: pH effects on the electrochemical reduction of CO (2) towards C 2 products on stepped copper
المؤلفون: Liu, Xinyan, Schlexer, Philomena, Xiao, Jianping, Ji, Yongfei, Wang, Lei, Sandberg, Robert B., Tang, Michael, Brown, Kristopher S., Peng, Hongjie, Ringe, Stefan, Hahn, Christopher, Jaramillo, Thomas F., Nørskov, Jens K., Chan, Karen
المصدر: Liu , X , Schlexer , P , Xiao , J , Ji , Y , Wang , L , Sandberg , R B , Tang , M , Brown , K S , Peng , H , Ringe , S , Hahn , C , Jaramillo , T F , Nørskov , J K & Chan , K 2019 , ' pH effects on the electrochemical reduction of CO (2) towards C 2 products on stepped copper ' , Nature Communications , vol. 10 , no. 1 , 32 . https://doi.org/10.1038/s41467-018-07970-9
سنة النشر: 2019
المجموعة: Technical University of Denmark: DTU Orbit / Danmarks Tekniske Universitet
الوصف: We present a microkinetic model for CO (2) reduction (CO (2) R) on Cu(211) towards C 2 products, based on energetics estimated from an explicit solvent model. We show that the differences in both Tafel slopes and pH dependence for C 1 vs C 2 activity arise from differences in their multi-step mechanisms. We find the depletion in C 2 products observed at high overpotential and high pH to arise from the 2nd order dependence of C-C coupling on CO coverage, which decreases due to competition from the C 1 pathway. We further demonstrate that CO (2) reduction at a fixed pH yield similar activities, due to the facile kinetics for CO 2 reduction to CO on Cu, which suggests C 2 products to be favored for CO 2 R under alkaline conditions. The mechanistic insights of this work elucidate how reaction conditions can lead to significant enhancements in selectivity and activity towards higher value C 2 products.
نوع الوثيقة: article in journal/newspaper
وصف الملف: application/pdf
اللغة: English
Relation: https://orbit.dtu.dk/en/publications/f7526c6e-8720-48e0-97f0-a35174d10b68
DOI: 10.1038/s41467-018-07970-9
الاتاحة: https://orbit.dtu.dk/en/publications/f7526c6e-8720-48e0-97f0-a35174d10b68
https://doi.org/10.1038/s41467-018-07970-9
https://backend.orbit.dtu.dk/ws/files/164554020/s41467_018_07970_9.pdf
Rights: info:eu-repo/semantics/openAccess
رقم الانضمام: edsbas.50389A1F
قاعدة البيانات: BASE
الوصف
DOI:10.1038/s41467-018-07970-9