固碳产甲烷微生物阴极能质传输特性数值模拟

doi:10.11949/0438-1157.20191600

摘要/Abstract

摘要：

固碳产甲烷微生物电合成系统以附着其电极表面的生物膜为催化剂，可以在处理废水的同时将CO₂转化为甲烷，极具应用前景。微生物阴极是该系统的核心部件之一，其表面生物膜内的能质传输特性极大地影响系统性能。针对微生物阴极能质传输特性尚不明确的问题，推导了微生物阴极电极反应动力学方程（Nernst-Monod方程），构建了耦合生化/电化学反应的物质传输理论模型，研究了不同阴极电势、生物膜电导率以及孔隙率对阴极生物膜内电荷及物质传输的影响规律。研究结果表明当阴极电势高于-0.5 V (vs SHE)时，随阴极电势的降低生物膜内电流密度增大，底物浓度降低；但当阴极电势降低至-0.5 V(vs SHE)后，生物膜消耗电子还原底物的能力几乎达到饱和；低电导率（<10^-3S/m）会导致生物膜内形成明显的电势差，使得底物利用速率降低，严重影响微生物阴极的性能；生物膜孔隙率控制在0.4时，微生物阴极可达到最佳电流密度。

关键词: 微生物电合成系统, 二氧化碳还原, 生物膜, 传质, 动力学模型

Abstract:

The carbon-fixing methanogenic microbial electrosynthesis system uses a biofilm attached to the surface of its electrode as a catalyst, which can convert CO₂into methane while treating wastewater, which has great application prospects. As one of the core components, the biocathode determines the performance of the system. Herein, we derived a Nernst-Monod equation applicable to biocathodes, and constructed a mathematical model of the electron and mass transfer within the biocathode. The effects of different biocathode potentials, biofilm conductivity, and biofilm porosity on transport characteristics of the biofilm are studied. The results showed that the current density within the biofilm increased, and the substrate concentration within the biofilm decreased towards the direction of electrode with the decreasing cathode potential when the potential > -0.5 V (vs SHE). On the other hand, the capability of biofilm consuming electrons was almost saturated when the cathode potential < -0.5 V(vs SHE). A low conductivity of the biofilm (<10^-3 S/m) could cause an obvious potential difference within the biofilm, reducing the substrate utilization rate and biocathode performance. When the biofilm porosity is controlled at 0.4, the microbial cathode can reach the optimal current density.

Key words: microbial electrosynthesis, carbon dioxide reduction, biofilm, mass transfer, kinetic modeling

中图分类号:

X 703

宋珣, 付乾, 李俊, 张亮, 廖强, 朱恂. 固碳产甲烷微生物阴极能质传输特性数值模拟[J]. 化工学报, 2020, 71(5): 2273-2282.

Xun SONG, Qian FU, Jun LI, Liang ZHANG, Qiang LIAO, Xun ZHU. Numerical simulation of transport characteristics in biocathodes catalyzing carbon dioxide to methane[J]. CIESC Journal, 2020, 71(5): 2273-2282.

图/表 8

图1 固碳产甲烷微生物电合成系统示意图

Fig.1 Schematic diagram of CH4-producing microbial electrosynthesis system

图2 几何模型计算区域示意图①阴极碳纸；②阴极生物膜；③浓度扩散层；④主体溶液

Fig.2 Schematic diagram of geometric model calculation area

表1 模型参数

Table 1 Parameters of model

参数

数值

参数来源

温度/K

生物膜厚度/μm

303.15

实验

浓度扩散层厚度/μm

100

[32]

主体溶液底物浓度/( mol/m³)

底物扩散系数/( m²/s)

半饱和常数/( mol/m³)

底物最大比反应速率/( mol/(kg·s))

电子受体电子当量

活性生物质电子当量

阴极生物膜电导率/( S/m)

生物膜平均密度/( kg/m³)

生物膜平均孔隙率

活性生物量内源呼吸系数/d^-1

29.76

1.2×10^-9

25.6

1.56×10^-4

0.177

0.0228

200

0.47

0.05

实验

[33]

实验

[18]

实验

[18]

[34]

[18]

图3 不同电势运行情况下微生物阴极电流密度

Fig.3 Current density of biocathodes operating at different potentials

图4 阴极电势对生物膜内电流密度及底物浓度的影响

Fig.4 Effect of cathode potential on current density and substrate concentration of biocathodes

图5 电导率对生物膜内电流密度、电势、底物浓度以及底物利用速率的影响

Fig.5 Effect of biofilm conductivity on current density, potential, substrate concentration, and substrate utilization rate

图6 生物膜孔隙率对底物浓度、电势及电流密度的影响

Fig.6 Effect of biofilm porosity on substrate concentration, potential, and current density

图7 孔隙率对底物浓度的影响以及生物膜内孔隙率、电导率、电势及电流密度的变化

Fig.7 Effect of porosity on substrate concentration, and varying of porosity, electrical conductivity, potential, and current density in biofilms

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