Boosting Electrocatalytic Nitrate Reduction through Enhanced Mass Transfer in Cu-Bipyridine 2D Covalent Organic Framework Films

被引:1
作者
Zhu, Ying [1 ]
Duan, Haiyan [1 ]
Gruber, Christoph G. [2 ]
Qu, Wenqiang [1 ]
Zhang, Hui [1 ]
Wang, Zhenlin [1 ]
Zhong, Jian [1 ]
Zhang, Xinhe [1 ]
Han, Lupeng [1 ]
Cheng, Danhong [1 ]
Medina, Dana D. [3 ,4 ]
Cortes, Emiliano [2 ]
Zhang, Dengsong [1 ]
机构
[1] Shanghai Univ, Innovat Inst Carbon Neutral, Coll Sci, Dept Chem,Int Joint Lab Catalyt Chem,State Key Lab, Shanghai 200444, Peoples R China
[2] Ludwig Maximilians Univ LMU, Fac Phys, Nanoinst Munich, D-80539 Munich, Germany
[3] Ludwig Maximilians Univ LMU, Dept Chem, D-81377 Munich, Germany
[4] Ludwig Maximilians Univ LMU, Ctr Nanosci CeNS, D-81377 Munich, Germany
基金
中国国家自然科学基金;
关键词
Catalytic interface; Nitrate reduction; Ammonia synthesis; Electrocatalysis; Covalent organic frameworks; NITROGEN REDUCTION; AMMONIA-SYNTHESIS; HIGH-EFFICIENCY; SINGLE ATOMS; ELECTROREDUCTION; CONVERSION; SURFACES; WATER;
D O I
10.1002/anie.202421821
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrocatalytic nitrate reduction (NO3RR) is a promising method for pollutant removal and ammonia synthesis and involves the transfer of eight electrons and nine protons. As such, the rational design of catalytic interfaces with enhanced mass transfer is crucial for achieving high ammonia yield rates and Faradaic efficiency (FE). In this work, we incorporated a Cu-bipyridine catalytic interface and fabricated crystalline 2D covalent organic framework films with significantly exposed catalytic sites, leading to improved FE and ammonia yield (FE=92.7 %, NH3 yield rate=14.9 mg & sdot; h-1cm-2 in 0.5 M nitrate) compared to bulk catalysts and outperforming most reported NO3RR electrocatalysts. The film-like morphology enhances mass transfer across the Cu-bipyridine interface, resulting in superior catalytic performance. We confirmed the reaction pathway and mechanism through in situ characterizations and theoretical calculations. The Cu sites act as primary centers for adsorption and activation, while the bipyridine sites facilitate water adsorption and dissociation, supplying sufficient H* and accelerating proton-coupled electron transfer kinetics. This study provides a viable strategy to enhance mass transfer at the catalytic interface through rational morphology control, boosting the intrinsic activity of catalysts in the NO3RR process.
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页数:12
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