CO2/C3H6O在金属氧化物耦合吡咯氮生物炭表面的共/竞吸附机理研究

汪辉春; 花昌豪; 陈萍; 顾明言; 龚成; 邹帅; 汪一

doi:10.19906/j.cnki.JFCT.2023059

CO₂/C₃H₆O在金属氧化物耦合吡咯氮生物炭表面的共/竞吸附机理研究

doi: 10.19906/j.cnki.JFCT.2023059

汪辉春^1,,
花昌豪^1,,
陈萍^1, ,,
顾明言^1,,
龚成^1,,
邹帅^1,,
汪一^2,

1.
安徽工业大学能源与环境学院, 安徽马鞍山 243002
2.
华中科技大学煤燃烧国家重点实验室, 湖北武汉 430074

基金项目: 国家自然科学基金青年项目（52206129），安徽省自然科学基金青年项目（2208085QE158）和煤燃烧国家重点实验室开放基金(FSKLCCA2206)

详细信息

通讯作者:
Tel:18395581520，E-mail:chp0109@126.com

中图分类号: TK6
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出版历程
- 收稿日期: 2023-06-16
- 修回日期: 2023-07-13
- 录用日期: 2023-07-20
- 网络出版日期: 2023-09-01

Study on co/competitive adsorption mechanism of CO₂/C₃H₆O on the surface of metal oxide-coupled pyrrole nitrogen biochar

WANG Huichun^1
,,
HUA Changhao^1
,,
CHEN Ping^{1
, ,},
GU Mingyan^1
,,
GONG Cheng^1
,,
ZOU Shuai^1
,,
WANG Yi^2
,

1.
School of Energy and Environment, Anhui University of Technology, Ma'anshan, 243002 Anhui, China
2.
State Key Laboratory of Energy Coal Combustion, Huazhong University of Science and Technology, Wuhan, 430074 Hubei, China

Funds: The project was supported by the National Natural Science Foundation of China Youth Program(52206129), Natural Science Foundation of Anhui Province(2208085QE158), State Key Laboratory of Coal Combustion Open Fund (FSKLCCA2206)

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Corresponding author: ．

摘要

摘要: 本研究采用密度泛函理论，通过比较吸附量、吸附能以及态密度和电荷差分密度的分析，探究了不同金属氧化物耦合吡咯氮生物炭(CN5@MO_x，MO_x = ZnO、CaO、Na₂O)表面CO₂与C₃H₆O(CO₂&C₃H₆O)的吸附机理。首先从CO₂/C₃H₆O单组分方面计算了其在CN5@MO_x表面吸附量和吸附能，计算结果显示在333 K、100 kPa时CN5@Na₂O表面对CO₂/C₃H₆O单组分吸附量分别为3.65、15.34 mmol/g，吸附能分别为−145.86、−132.47 kJ/mol，均高于CO₂/C₃H₆O单组分在CN5@CaO及CN5@ZnO表面吸附。得出Na₂O掺杂吡咯氮生物炭对CO₂/C₃H₆O单组分吸附效果最优。进一步研究了CO₂&C₃H₆O在CN5@MO_x表面共/竞吸附情况及机理。计算结果表明，CO₂&C₃H₆O在CN5@Na₂O、CN5@CaO、CN5@ZnO表面吸附存在临界温度(分别为333、353、393 K)，超过临界温度以后CO₂&C₃H₆O共存体系在CN5@MO_x表面吸附量较CO₂/C₃H₆O单组分有所提高。CO₂&C₃H₆O在CN5@Na₂O、CN5@CaO、CN5@ZnO表面吸附能分别比CO₂或C₃H₆O单组分吸附时至少高141.59、112.77、31.75 kJ/mol，CN5@MO_x表面对CO₂和C₃H₆O的吸附表现为协同促进作用，且CN5@Na₂O对CO₂&C₃H₆O共同吸附效果最佳。最后采用电荷差分密度和态密度分析CO₂&C₃H₆O在CN5@MO_x表面协同吸附作用机理，得出CO₂的吸附作用力是通过C₃H₆O与CO₂的间接相互作用产生的，Na₂O中Na与C₃H₆O电子云重叠，发生电荷转移，增强了两者间相互作用力，CN5@Na₂O表面C₃H₆O与CN5在p轨道主要共振峰结合能较CN5@ZnO低了3.43 eV，使得C₃H₆O在CN5@Na₂O表面吸附最稳定。
- 吡咯氮生物炭 /
- 金属氧化物 /
- CO₂ /
- C₃H₆O
Abstract: Biomass has a wide range of sources and is porous, and it is a raw material for the preparation of adsorbents with high application value. The adsorption effect of metal oxide-modified biochar on CO₂ and acetone can be significantly improved, but the together/competitive relationship and adsorption mechanism of metal oxide-modified biomass-based adsorbent for simultaneous adsorption of multiple components are not clear. Based on this, the co-adsorption relationship between CO₂ and C₃H₆O on the surface of metal oxide-doped nitrogen-rich biochar was carried out, which is of great significance for the multi-component synergistic adsorption and removal of biomass-based adsorbents. In this study, the adsorption mechanism of CO₂ and C₃H₆O (CO₂ & C₃H₆O) on the surface of different metal oxide-coupled pyrrole biochar (CN5 @ MO_x, MO_x = ZnO, CaO, Na₂O) was explored by comparing the adsorption capacity, adsorption energy, state density and charge differential density analysis.Firstly, the adsorption capacity and adsorption energy of CO₂/C₃H₆O single component were calculated from the CN5 @ MO_x surface, and the calculation results show that at 333 K and 100 kPa, the adsorption capacity of CO₂/C₃H₆O on the surface of the CN5 @ Na₂O is 3.65 mmol/g and 15.34 mmol/g, and the adsorption energy is −145.86 kJ/mol and −132.47 kJ/mol, respectively, which are higher than that of CO₂/C₃H₆O on the surface of CN5 @ CaO and CN5 @ ZnO.It was concluded that Na₂O-doped pyrrole-nitrogen biochar had the best adsorption effect on CO₂/C₃H₆O one-component adsorption. The common/competitive adsorption of CO₂ & C₃H₆O on the CN5 @ MO_x surface was further studied. The calculation results show that there are critical temperatures for the adsorption of CO₂ & C₃H₆O on the surface of CN5 @ Na₂O, CN5 @ CaO and CN5 @ ZnO(333 K, 353 K and 393 K, respectively), and the adsorption capacity of CO₂ & C₃H₆O coexistence system on the CN5 @ MO_x surface is higher than that of CO₂/C₃H₆O single component after the critical temperature. The adsorption energy of CO₂ & C₃H₆O on the surface of CN5 @ Na₂O, CN5 @ CaO and CN5 @ ZnO was at least 141.59 kJ/mol, 112.77 kJ/mol and 31.75 kJ/mol higher than that of CO₂ or C₃H₆O single-component adsorption, respectively, and the adsorption of CO₂ and C₃H₆O on the CN5 @ MO_x surface showed a synergistic promotion effect, and the CN5 @ Na₂O had the best co-adsorption effect on CO₂ & C₃H₆O.Finally, the electron density difference and density of state were used to analyze the mechanism of synergistic adsorption of CO₂ & C₃H₆O on the CN5 @ MO_x surface, and it was concluded that the adsorption force of CO₂ was generated by the indirect interaction between C₃H₆O and CO₂, and the electron cloud of Na and C₃H₆O in Na₂O overlapped, and charge transfer occurred, which enhanced the interaction force between the two. The binding energy of the main formant of C₃H₆O and CN5 in the p orbital on the CN5 @ Na₂O surface is 3.43 eV lower than that of CN5 @ ZnO, making the most stable adsorption of C₃H₆O on the CN5 @ Na₂O surface.
- pyrrole functional biochar /
- metal oxides /
- co₂ /
- c₃h₆o

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图 1 C-N5片段

Figure 1 C-H, C-N5 fragments

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图 2 不同生物质炭优化后的构型

Figure 2 Optimized configuration of different biochars

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图 3 CN5、CN5@MO_x构型孔径分布

Figure 3 CN5, CN5@MO_x configuration pore size distribution

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图 4 CN5与ZnO在Top、Bridge、Hollow位点耦合构型

Figure 4 CN5 and ZnO are coupled at the Top, Bridge and Hollow sites

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图 5 CN5与ZnO不同耦合位点吸附CO₂

Figure 5 CN5 adsorbs CO₂ at different coupling sites with ZnO

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图 6 吸附量随温度的变化

Figure 6 Adsorption capacity varies with temperature

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图 7 C₃H₆O在不同金属氧化物耦合含吡咯氮生物质炭表面的吸附构型

Figure 7 Adsorption configuration of C₃H₆O on the surface of pyrrole nitroza-containing biochar coupled with different metal oxides

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图 8 (a)、(b)、(c)分别为C₃H₆O在不同生物质炭表面吸附电荷差分密度图

Figure 8 (a), (b) and (c) were the differential density maps of C₃H₆O adsorbed charges on different biochar surfaces (blue and yellow regions gained and lost electrons, respectively)

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图 9 C₃H₆O在CN5@MO_x表面的PDOS谱图

Figure 9 PDOS diagram of C₃H₆O on the surface of the CN5@MO_x

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图 10 CO₂在不同金属氧化物耦合含吡咯氮生物质炭表面的吸附构型

Figure 10 Adsorption configuration of CO₂ coupled with pyrrole nitrogen-containing biochar in different metal oxides

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图 11 (a)、(c)、(e)、(h)为吸附电荷差分密度图;(b)、(d)、(f)、(g)、(i)、(j)为剖面图

Figure 11 (a), (c), (e), (h) are the differential density diagram of the adsorption charge; (b), (d), (f), (g), (i), (j) are the profile diagrams(blue and red areas gain and loss of electrons, respectively)

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图 12 CO₂&C₃H₆O在CN5@ZnO、CN5@CaO、CN5@Na₂O上吸附PDOS谱图

Figure 12 CO₂&C₃H₆O adsorbed PDOS on CN5@ZnO, CN5@CaO and CN5@Na₂O

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表 1 CN5、CN5@MO_x构型比表面积和孔容

Table 1 CN5, CN5@MO_x configuration specific surface area(S_BET) and pore volume(v_Total)

Sample	S_BET/(m²·g⁻¹)	v_Total/(cm³·g⁻¹)
CN5	1803.37	0.70
CN5@ZnO	1912.31	0.83
CN5@CaO	1576.90	0.69
CN5@Na₂O	1678.84	0.68

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表 2 CN5与ZnO不同耦合位点优化平衡能量

Table 2 CN5 and ZnO have different coupling sites to optimize the balance energy

Coupling site	Balance energy/eV
Top	−74207.0723
Bridge	−74207.1353
Hollow	−74207.2676

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表 3 CN5与ZnO不同耦合位点对CO₂吸附能(E_ads)

Table 3 CN5 and ZnO have different coupling sites for CO₂ adsorption energy(E_ads)

Coupling site	E_ads/eV	E_ads/(kJ·mol⁻¹)
Top	−1.23	−119.05
Bridge	−1.20	−116.19
Hollow	−1.15	−111.05

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表 4 C₃H₆O的吸附能

Table 4 Calculation results of adsorption energy of C₃H₆O

Structure	E_ads/eV	E_ads/(kJ·mol⁻¹)
CN5@ZnO	−0.14944	−14.42
CN5@CaO	−0.50754	−48.97
CN5@Na₂O	−1.37294	−132.47

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表 5 CO₂/C₃H₆O吸附能

Table 5 Calculation results of CO₂/C₃H₆O adsorption energy

Structure	Eads/(kJ·mol⁻¹)
	CO₂	C₃H₆O	CO₂&C₃H₆O
	CO₂	C₃H₆O	CO₂//C₃H₆O	C₃H₆O⊥CO₂	CO₂⊥C₃H₆O
CN5@ZnO	−120.88	−14.42	−138.63	−140.21	−152.63
CN5@CaO	−133.04	−48.97	−161.99	−245.81	−168.58
CN5@Na₂O	−145.86	−132.47	−242.82	−285.86	−287.45

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