Microkinetic modeling has drawn increasing attention for quantitatively analyzing catalytic networks in recent decades, in which the speed and stability of the solver play a crucial role. However, for the multi-step complex systems with a wide variation of rate constants, the often encountered stiff problem leads to the low success rate and high computational cost in the numerical solution. Here, we report a new efficient sensitivity-supervised interlock algorithm (SSIA), which enables us to solve the steady state of heterogeneous catalytic systems in the microkinetic modeling with a 100% success rate. In SSIA, we introduce the coverage sensitivity of surface intermediates to monitor the low-precision time-integration of ordinary differential equations, through which a quasi-steady-state is located. Further optimized by the high-precision damped Newton’s method, this quasi-steady-state can converge with a low computational cost. Besides, to simulate the large differences (usually by orders of magnitude) among the practical coverages of different intermediates, we propose the initial coverages in SSIA to be generated in exponential space, which allows a larger and more realistic search scope. On examining three representative catalytic models, we demonstrate that SSIA is superior in both speed and robustness compared with its traditional counterparts. This efficient algorithm can be promisingly applied in existing microkinetic solvers to achieve large-scale modeling of stiff catalytic networks.
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14 January 2021
Research Article|
January 11 2021
SSIA: A sensitivity-supervised interlock algorithm for high-performance microkinetic solving
Jianfu Chen
;
Jianfu Chen
1
Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
, 130 Meilong Road, Shanghai 200237, People’s Republic of China
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Menglei Jia;
Menglei Jia
1
Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
, 130 Meilong Road, Shanghai 200237, People’s Republic of China
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Zhuangzhuang Lai;
Zhuangzhuang Lai
1
Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
, 130 Meilong Road, Shanghai 200237, People’s Republic of China
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Peijun Hu
;
Peijun Hu
1
Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
, 130 Meilong Road, Shanghai 200237, People’s Republic of China
2
School of Chemistry and Chemical Engineering, The Queen’s University of Belfast
, Belfast BT9 5AG, United Kingdom
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Haifeng Wang
Haifeng Wang
a)
1
Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
, 130 Meilong Road, Shanghai 200237, People’s Republic of China
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 154, 024108 (2021)
Article history
Received:
October 07 2020
Accepted:
December 18 2020
Citation
Jianfu Chen, Menglei Jia, Zhuangzhuang Lai, Peijun Hu, Haifeng Wang; SSIA: A sensitivity-supervised interlock algorithm for high-performance microkinetic solving. J. Chem. Phys. 14 January 2021; 154 (2): 024108. https://doi.org/10.1063/5.0032228
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