scholarly journals Rational design of a bi-functional mononuclear Cobalt-dependent composite with improved catalytic activity and excellent durability for the oxygen reduction reaction

Author(s):  
Behnam Seyyedi ◽  
Bafrin Shakhseh
2019 ◽  
Author(s):  
Liang Cao ◽  
Le, Niu ◽  
Tim Mueller

To facilitate the rational design of alloy catalysts, we introduce a method for rapidly calculating the structure and catalytic properties of a substitutional alloy surface that is in equilibrium with the underlying bulk phase. We implement our method by developing a way to generate surface cluster expansions that explicitly account for the lattice parameter of the bulk structure. This approach makes it possible to computationally map the structure and catalytic activity of an alloy surface at every point in the alloy phase diagram, enabling the identification of synthesis conditions likely to result in highly active catalysts. We demonstrate our approach by analyzing Pt-rich Pt–Ni catalysts for the oxygen reduction reaction, finding two regions in the phase diagram that are predicted to result in highly active catalysts. Our analysis indicates that the Pt<sub>3</sub>Ni(111) surface, which has the highest known specific activity for the oxygen reduction reaction, is likely able to achieve its high activity through the formation of an intermetallic phase with L1<sub>2</sub> order. We use the generated surface structure and catalytic activity maps to demonstrate how the intermetallic nature of this phase leads to high catalytic activity and discuss how the underlying principles can be used in catalysis design. We further discuss the importance of surface phases and demonstrate how they can dramatically affect catalytic activity.


2019 ◽  
Author(s):  
Liang Cao ◽  
Le, Niu ◽  
Tim Mueller

To facilitate the rational design of alloy catalysts, we introduce a method for rapidly calculating the structure and catalytic properties of a substitutional alloy surface that is in equilibrium with the underlying bulk phase. We implement our method by developing a way to generate surface cluster expansions that explicitly account for the lattice parameter of the bulk structure. This approach makes it possible to computationally map the structure and catalytic activity of an alloy surface at every point in the alloy phase diagram, enabling the identification of synthesis conditions likely to result in highly active catalysts. We demonstrate our approach by analyzing Pt-rich Pt–Ni catalysts for the oxygen reduction reaction, finding two regions in the phase diagram that are predicted to result in highly active catalysts. Our analysis indicates that the Pt<sub>3</sub>Ni(111) surface, which has the highest known specific activity for the oxygen reduction reaction, is likely able to achieve its high activity through the formation of an intermetallic phase with L1<sub>2</sub> order. We use the generated surface structure and catalytic activity maps to demonstrate how the intermetallic nature of this phase leads to high catalytic activity and discuss how the underlying principles can be used in catalysis design. We further discuss the importance of surface phases and demonstrate how they can dramatically affect catalytic activity.


2017 ◽  
Vol 5 (42) ◽  
pp. 22163-22169 ◽  
Author(s):  
Baolong Zhou ◽  
Liangzhen Liu ◽  
Pingwei Cai ◽  
Guang Zeng ◽  
Xiaoqiang Li ◽  
...  

Two nitrogen-rich porous organic polymers (POPs) were prepared via Schiff base chemistry. Carbonization of these POPs results in porous carbon nanohybrids which exhibit excellent catalytic activity toward the oxygen reduction reaction (ORR).


2016 ◽  
Vol 120 (40) ◽  
pp. 22895-22902 ◽  
Author(s):  
Xuecheng Cao ◽  
Tao Hong ◽  
Ruizhi Yang ◽  
Jing-Hua Tian ◽  
Changrong Xia ◽  
...  

2013 ◽  
Vol 17 (04) ◽  
pp. 252-258 ◽  
Author(s):  
Qinggang He ◽  
Xiao Cheng ◽  
Ying Wang ◽  
Ruimin Qiao ◽  
Wanli Yang ◽  
...  

The dicobalt complex [ Co2(L2) ] of a Schiff-base pyrrole macrocycle adopts a Pacman structure in solution and the solid state and shows much greater catalytic activity and selectivity for the four-electron oxygen reduction reaction (ORR) than the mononuclear cobalt phthalocyanine (CoPc) counterpart. Soft X-ray absorption spectroscopy (XAS) shows that the Co center in Co2(L2) is of the same valence as mononuclear CoPc . However, the former complex shows higher unoccupied Co 3d density which is believed to be beneficial for electron transfers. Furthermore, the XAS data suggests that the crystal fields for Co2(L2) and CoPc are different, and that an interaction remains between two Co atoms in Co2(L2) . DFT calculations imply that the sterically hindered, cofacial structure of the dicobalt complex is critical for the operation of the four-electron reaction pathway during the ORR.


2022 ◽  
Author(s):  
Huixin Ma ◽  
Daijie Deng ◽  
Honghui Zhang ◽  
Feng Chen ◽  
Junchao Qian ◽  
...  

Nitrogen-coordinated single-atom manganese in multi-dimensional nitrogen-doped carbon electrocatalysts (Mn-NC) was successful constructed by combing two-dimensional nanosheets and one-dimensional nanofibers. The Mn-NC exhibited excellent oxygen reduction reaction catalytic activity with half-wave...


2021 ◽  
Author(s):  
Binhong He ◽  
Yangyang Chen ◽  
Da Hu ◽  
Ziyan Wen ◽  
Minjie Zhou ◽  
...  

Rational design of oxygen reduction reaction (ORR) electrocatalysts is essential for promoting the development of clean energy conversion devices. Herein, we report an in–situ sacrificial template strategy combining with external...


Catalysts ◽  
2021 ◽  
Vol 11 (10) ◽  
pp. 1163
Author(s):  
Ning Cui ◽  
Kexiao Bi ◽  
Wei Sun ◽  
Qianqian Wu ◽  
Yinan Li ◽  
...  

MOF–derived porous carbon is a type of promising catalyst to replace expensive Pt–based catalysts for oxygen reduction reaction (ORR). The catalytic activity for ORR depends closely on pyrolysis conditions. In this work, a Co–doped ZIF–8 material was chosen as a research object. The effect of pyrolysis conditions (temperature, heating rate, two–step heating) on the ORR performance of ZIF–derived carbon catalysts was systematically studied. The Co–ZIF–8 catalyst carbonized at 900 °C exhibits better ORR catalytic activity than that carbonized at 800 °C and 1000 °C. Moreover, a low heating rate can enhance catalytic activity. Two–step pyrolysis is proven to be an effective way to improve the performance of catalysts. Reducing the heating rate in the low–temperature stage is more beneficial to the ORR performance, compared to the heating rate in the high–temperature stage. The results show that the Co–ZIF–8 catalyst exhibits the best performance when the precursor was heated to 350 °C at 2 °C/min, and then heated to 900 °C at 5 °C/min. The optimum Co–ZIF–8 catalyst shows a half–wave potential of 0.82 V and a current density of 5.2 mA·cm−2 in 0.1 M KOH solution. It also exhibits high content of defects and good graphitization. TEM mapping shows that Co and N atoms are highly dispersed in the polyhedral carbon skeleton. However, two–step pyrolysis has no significant effect on the stability of the catalyst.


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