Boosting oxygen reduction catalysis with abundant copper single atom active sites

2018 ◽  
Vol 11 (8) ◽  
pp. 2263-2269 ◽  
Author(s):  
Feng Li ◽  
Gao-Feng Han ◽  
Hyuk-Jun Noh ◽  
Seok-Jin Kim ◽  
Yalin Lu ◽  
...  

Single atomic copper doping in ultrathin nitrogenated carbon nanosheets over 20.9 wt% was achieved, greatly boosting the oxygen reduction catalysis.

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Guokang Han ◽  
Xue Zhang ◽  
Wei Liu ◽  
Qinghua Zhang ◽  
Zhiqiang Wang ◽  
...  

AbstractSingle-atom catalysts are becoming increasingly significant to numerous energy conversion reactions. However, their rational design and construction remain quite challenging due to the poorly understood structure–function relationship. Here we demonstrate the dynamic behavior of CuN2C2 site during operando oxygen reduction reaction, revealing a substrate-strain tuned geometry distortion of active sites and its correlation with the activity. Our best CuN2C2 site, on carbon nanotube with 8 nm diameter, delivers a sixfold activity promotion relative to graphene. Density functional theory and X-ray absorption spectroscopy reveal that reasonable substrate strain allows the optimized distortion, where Cu bonds strongly with the oxygen species while maintaining intimate coordination with C/N atoms. The optimized distortion facilitates the electron transfer from Cu to the adsorbed O, greatly boosting the oxygen reduction activity. This work uncovers the structure–function relationship of single-atom catalysts in terms of carbon substrate, and provides guidance to their future design and activity promotion.


2020 ◽  
Vol MA2020-01 (38) ◽  
pp. 1688-1688
Author(s):  
Jing Liu ◽  
JeongHan Roh ◽  
DongHoon Song ◽  
Junu Bak ◽  
Hyo-Jong Kim ◽  
...  

2020 ◽  
Vol 2 (12) ◽  
pp. 5769-5776
Author(s):  
Qingyu Li ◽  
Dingding Kong ◽  
Xinyi Zhao ◽  
Yezheng Cai ◽  
Zhaoling Ma ◽  
...  

Selectively creating active sites that can work well in different media as much as possible remains an open challenge for the widespread application of sustainable metal air batteries and fuel cells.


2020 ◽  
Vol 13 (9) ◽  
pp. 2856-2863 ◽  
Author(s):  
Zhuoli Jiang ◽  
Tao Wang ◽  
Jiajing Pei ◽  
Huishan Shang ◽  
Danni Zhou ◽  
...  

We discover that an Sb single atom material consisting of Sb–N4 moieties anchored on N-doped carbon nanosheets can serve as a CO2RR catalyst to produce formate with high efficiency.


Research ◽  
2019 ◽  
Vol 2019 ◽  
pp. 1-12 ◽  
Author(s):  
Dong-Li Meng ◽  
Chun-Hui Chen ◽  
Jun-Dong Yi ◽  
Qiao Wu ◽  
Jun Liang ◽  
...  

It is highly desired but challenging to achieve highly active single-atom Fe sites from iron-based metal-organic frameworks (MOFs) for efficient oxygen reduction reaction (ORR) due to the easy aggregation of iron species and formation of the inactive Fe-based particles during pyrolysis. Herein, a facile migration-prevention strategy is developed involving the incorporation of polyaniline (PANI) into the pores of iron porphyrinic-based MOF PCN-224(Fe) and followed by pyrolysis to obtain the single-atom Fe implanted N-doped porous carbons material PANI@PCN-224(Fe)-900. The introduced PANI inside the pores of PCN-224(Fe) not only served as protective fences to prevent the aggregation of the iron species during thermal annealing, but also acted as nitrogen sources to increase the nitrogen content and form Fe-Nx-C active sites. Compared with the pristine PCN-224(Fe) derived carbonization sample containing Fe-based particles, the carbonaceous material PANI@PCN-224(Fe)-900 without inactive Fe-based particles exhibited superb ORR electrocatalytic activity with a more positive half-wave potential, significantly improved stability in both alkaline media, and more challenging acidic condition. The migration-prevention strategy provides a new way to fabricate atomically dispersed metal active sites via pyrolysis approach for promoting catalysis.


2020 ◽  
Vol 31 (16) ◽  
pp. 165401 ◽  
Author(s):  
Qian Ke ◽  
Liu Yang ◽  
Yubei Gao ◽  
Xi-Lin Wu ◽  
Feng Chen ◽  
...  

2020 ◽  
Vol 8 (20) ◽  
pp. 10193-10198 ◽  
Author(s):  
Xiyu Li ◽  
Sai Duan ◽  
Edward Sharman ◽  
Yuan Zhao ◽  
Li Yang ◽  
...  

Both a linear OER activity trend that reaches an ideal 0 V overpotential and a new volcano ORR activity trend with the volcano apex around ideal 1.23 V limiting potential are associated with our dual-active-site designs.


Research ◽  
2020 ◽  
Vol 2020 ◽  
pp. 1-51 ◽  
Author(s):  
Junxing Han ◽  
Juanjuan Bian ◽  
Chunwen Sun

Oxygen reduction reaction (ORR) plays significant roles in electrochemical energy storage and conversion systems as well as clean synthesis of fine chemicals. However, the ORR process shows sluggish kinetics and requires platinum-group noble metal catalysts to accelerate the reaction. The high cost, rare reservation, and unsatisfied durability significantly impede large-scale commercialization of platinum-based catalysts. Single-atom electrocatalysts (SAECs) featuring with well-defined structure, high intrinsic activity, and maximum atom efficiency have emerged as a novel field in electrocatalytic science since it is promising to substitute expensive platinum-group noble metal catalysts. However, finely fabricating SAECs with uniform and highly dense active sites, fully maximizing the utilization efficiency of active sites, and maintaining the atomically isolated sites as single-atom centers under harsh electrocatalytic conditions remain urgent challenges. In this review, we summarized recent advances of SAECs in synthesis, characterization, oxygen reduction reaction (ORR) performance, and applications in ORR-related H2O2 production, metal-air batteries, and low-temperature fuel cells. Relevant progress on tailoring the coordination structure of isolated metal centers by doping other metals or ligands, enriching the concentration of single-atom sites by increasing metal loadings, and engineering the porosity and electronic structure of the support by optimizing the mass and electron transport are also reviewed. Moreover, general strategies to synthesize SAECs with high metal loadings on practical scale are highlighted, the deep learning algorithm for rational design of SAECs is introduced, and theoretical understanding of active-site structures of SAECs is discussed as well. Perspectives on future directions and remaining challenges of SAECs are presented.


2020 ◽  
Vol 11 (4) ◽  
pp. 1404-1410 ◽  
Author(s):  
Yaodan Zhou ◽  
Wen Yang ◽  
Wellars Utetiwabo ◽  
Yi-meng Lian ◽  
Xue Yin ◽  
...  

2021 ◽  
Vol 490 ◽  
pp. 229483
Author(s):  
Haipeng Liu ◽  
Shengli Zhu ◽  
Zhenduo Cui ◽  
Zhaoyang Li ◽  
Shuilin Wu ◽  
...  

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