Experimental and DFT Studies of Influence of Flue Gas Components on the Interaction between CaO and As during Sludge Combustion
Abstract
:1. Introduction
2. Materials
3. Experimental Setup
3.1. Combustion Experiments
3.2. Methods
4. Theoretical Calculations
4.1. Calculation Parameters
4.2. Model Parameters
4.3. Calculation of Adsorption Energy
5. Results and Discussion
5.1. Migration Behaviour of As from Sludge Combustion Process
5.1.1. Impact of CaO on As Migration Pattern
5.1.2. Impact of CO2/SO2/H2O on the Interaction of CaO and As
5.2. Characterization Analysis
5.2.1. Porosity Structure Analysis
5.2.2. Microscopic Morphological Analysis
5.2.3. Phase Composition Analysis
5.3. Calculation Results and Discussion
6. Discussion
- (1)
- CaO chemically reacted with gaseous arsenic-containing compounds to produce more stable calcium-arsenic compounds, and CaO immobilized As better than CaSO4. CO2 contributed significantly to the immobilization of As. When CO2 concentration increased from 0% to 30%, the residual rates of As increased by 6.33%. SO2 was detrimental to the immobilization of As. As SO2 concentration increased from 0% to 0.2%, the residual rate of As showed a decreasing trend, decreasing by 16.76%. H2O had a significant inhibitory effect on the immobilization of As. The moisture content in sludge increased from 0% to 30%, and the residual rate of As was decreased by 29.38%.
- (2)
- The residual rate of As after combustion of sludge loaded with 4% CaO in 20CO2/20O2/60N2 atmosphere increased by 1.09%, and CO2 favored the capture of As by CaO. The residual rate of As was reduced by 8.96% after combustion of sludge loaded with 4% CaO in 0.15SO2/20O2/79.85N2 atmosphere, and SO2 inhibited CaO to fix As. The residual rate of As was reduced by 8.89% at 20% water content in sludge loaded with 4% CaO, and the presence of water was unfavorable for the capture of As by CaO.
- (3)
- DFT calculations showed that the CaO(001) surface O top site was the active site for the adsorption of As2O3, CO2, SO2, and H2O molecules. The adsorption energy of As2O3 molecules at the OC1 top site (−209.972 kJ/mol) was higher than at the Osurf top site (−202.774 kJ/mol). CO2 favored the stable adsorption of As2O3 molecules at the OC1 top site to the detriment of their adsorption at the top sites of OC0, OC2, and OC3. The adsorption energies of As2O3 molecules at potential active sites on SO2+CaO(001) surface were all lower than those on clean CaO(001) surface, and SO2 was unfavorable for the adsorption of As2O3 molecules at the top sites of OS0~OS4. For the OH0 and OH2 top sites, the H-OH bonds in the H2O molecule were broken, and the resulting OH atoms underwent more intense orbital hybridization with the As atoms in the As2O3 molecule. The adsorption energies (−241.446 kJ/mol and −236.457 kJ/mol) of the stabilized structure after adsorption were higher than those of the Osurf top site, which greatly facilitated the stabilized adsorption of the As2O3 molecule, whereas the OH1 top site was not conducive to the stabilized adsorption of the As2O3 molecule. In addition, in the theoretical calculation section only considered As2O3 (g), a major form of As present in combustion flue gas. In the actual combustion process, there were also singlet, chlorinated states, etc., which needed to be further investigated in the follow-up work.
- (4)
- Migration was a complex physicochemical reaction during the actual combustion of sludge. When exploring the migration law, not only shall we analyze the influence of physical properties such as pore structure and changes in chemical forms such as compounds on the migration of As from a macroscopic point of view by means of experimental characterization, but we shall also explain the changes in the electronic structure of atoms and molecules as well as the changes in the adsorption energy from a microchemical point of view by means of theoretical calculations. Probing the migration pattern of As was instructive for the efficient removal of heavy metals from sludge and the realization of stable and clean combustion of sludge.
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
Appendix A
Adsorption Structures | Eads (kJ/mol) | As-Osurf Key Length (Å) | As-Osurf Population | q(As2O3) (e) | |
---|---|---|---|---|---|
As-terminus | 1-a | −202.533 | 1.836 | 0.32 | −0.39 |
2-a | −202.774 | 1.836 | 0.32 | −0.38 | |
3-a | 6.946 | - | - | −0.10 | |
4-a | 11.992 | - | - | −0.07 | |
O-terminus | 1-b | −202.273 | 1.836 | 0.32 | −0.38 |
2-b | 21.120 | - | - | 0.01 | |
3-b | −202.755 | 1.836 | 0.32 | −0.32 | |
4-b | −6.909 | - | - | −0.01 | |
As-O bond | 1-c | −31.735 | - | - | −0.17 |
2-c | −202.234 | 1.835 | 0.32 | −0.38 | |
3-c | −202.427 | 1.837 | 0.32 | −0.38 | |
4-c | −202.389 | 1.835 | 0.32 | −0.38 |
Adsorption Structure | Eads (kJ/mol) | C-Osurf Bond Length (Å) | C-Osurf Population | q(CO2) (e) | |
---|---|---|---|---|---|
C-terminus parallel | 1-a | −0.341 | - | - | −0.05 |
2-a | −123.321 | 1.393 | 0.63 | −0.64 | |
3-a | −123.379 | 1.392 | 0.63 | −0.64 | |
4-a | 16.863 | - | - | −0.01 |
Adsorption Structure | Eads (kJ/mol) | S-Osurf Bond Length (Å) | S-Osurf Population | q(SO2) (e) | |
---|---|---|---|---|---|
S-terminus parallel | 1-a | −169.444 | 1.699 | 0.21 | −0.31 |
2-a | −169.415 | 1.700 | 0.21 | −0.31 | |
3-a | −177.037 | 1.672 | 0.22 | −0.30 | |
4-a | 8.205 | - | - | −0.15 | |
S-terminus vertical | 1-b | −177.056 | 1.671 | 0.22 | −0.30 |
2-b | −169.502 | 1.698 | 0.21 | −0.31 | |
3-b | −176.661 | 1.672 | 0.23 | −0.3 | |
4-b | 8.195 | - | - | −0.1 |
Adsorption Structure | Eads (kJ/mol) | H-Osurf Bond Length (Å) | H-Osurf Population | q(H2O) (e) | |
---|---|---|---|---|---|
O-terminus parallel | 1-a | −58.875 | - | - | −0.25 |
2-a | 11.772 | - | - | −0.03 | |
3-a | −77.699 | 1.036 | 0.48 | −0.26 | |
4-a | −58.537 | - | - | −0.25 | |
O-terminus vertical | 1-b | 18.005 | - | - | 0.01 |
2-b | 19.182 | - | - | 0 | |
3-b | −8.606 | - | - | 0.03 | |
4-b | −4.766 | - | - | 0.03 |
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Proximate Analysis (%) | Ultimate Analysis (%) | |||||||
---|---|---|---|---|---|---|---|---|
Mad | Aad | Vad | FCad | Cd | Hd | Od | Nd | Sd |
2.53 | 49.67 | 43.03 | 4.77 | 23.45 | 3.51 | 17.14 | 4.35 | 0.58 |
Heavy Metals (mg/kg) | Minerals (%) | ||||
---|---|---|---|---|---|
As | SiO2 | CaO | Al2O3 | P2O5 | MgO |
15.025 | 32.732 | 16.992 | 17.14 | 7.680 | 7.639 |
Combustion Conditions | Temperature (°C) | Combustion Atmosphere (vol.%) | Samples (2 g) |
---|---|---|---|
T1 | 700 °C | 20O2/80N2 | 100% Sludge |
T2 | 800 °C | ||
T3 | 900 °C | ||
T4 | 1000 °C | ||
TC1 | 700 °C | 96% Sludge + 4% CaO | |
TC2 | 800 °C | ||
TC3 | 900 °C | ||
TC4 | 1000 °C | ||
TCS1 | 700 °C | 96% Sludge + 4% CaSO4 | |
TCS2 | 800 °C | ||
TCS3 | 900 °C | ||
TCS4 | 1000 °C | ||
C1 | 900 °C | 10CO2/20O2/70N2 | 100% Sludge |
C2 | 20CO2/20O2/60N2 | ||
C3 | 30CO2/20O2/50N2 | ||
C4 | 20CO2/20O2/60N2 | 96% Sludge + 4% CaO | |
S1 | 0.1SO2/20O2/79.9N2 | 100% Sludge | |
S2 | 0.15SO2/20O2/79.85N2 | ||
S3 | 0.2SO2/20O2/79.8N2 | ||
S4 | 0.15SO2/20O2/79.85N2 | 96% Sludge + 4% CaO | |
H1 | 20O2/80N2 | 10% H2O + 90% Sludge | |
H2 | 20% H2O + 80% Sludge | ||
H3 | 30% H2O + 70% Sludge | ||
H4 | 20% H2O + 76% Sludge + 4% CaO |
Device | Make | Type | Measuring | Accuracy |
---|---|---|---|---|
ICP-MS | Agilent (Beijing, China) | Agilent 7800 | ppb~ppm | 1–5% |
BET | Micromeritics (Beijing, China) | ASAP-2460 | 0.01 m2/g~1000 m2/g | 1–5% |
XRD | Malvern Panalytical (Beijing, China) | Panalytical Empyrean | 5°~85° | 1–5% |
SEM-EDS | ZEISS (Beijing, China) | ZEISS Sigma 300 | μm~nm | 1–5% |
Model | Key Length/Key Angle | Optimize Value (Å/°) | Reference Value (Å/°) | Relative Error (%) |
---|---|---|---|---|
CaO | a = b = c | 4.91 | 4.81 | 2.16 |
α = β = γ | 90.00 | 90.00 | 0.00 | |
CO2 | C-O | 1.17 | 1.16 | 0.86 |
O-C-O | 179.99 | 180.00 | 0.01 | |
SO2 | S-O | 1.46 | 1.43 | 1.89 |
O-S-O | 119.48 | 119.50 | 0.02 | |
H2O | H-O | 0.98 | 0.96 | 1.88 |
H-O-H | 103.74 | 104.50 | 0.73 | |
As2O3 | As-O | 1.87 | 1.86 | 0.43 |
As-O-As | 75.41 | 73.50 | 2.60 |
Samples | Specific Surface Area (m2/g) | Pore Volume (×10−2 cm3/g) |
---|---|---|
Sludge | 8.03 | 2.05 |
CaO | 7.13 | 1.33 |
T3 | 4.82 | 0.84 |
TC3 | 6.32 | 1.11 |
C4 | 5.86 | 1.02 |
S4 | 2.26 | 0.42 |
H4 | 3.52 | 0.51 |
Adsorption Structure | EadS (kJ·mol−1) | As-OX Bond Length (Å) | As-OX Population | q(As2O3) (e) | X-Osurf Key Length (Å) | X-Osurf Population | q(X) (e) |
---|---|---|---|---|---|---|---|
OC0 | −26.737 | - | - | −0.1 | 1.366 | 0.68 | −0.64 |
OC1 | −209.972 | 1.857 | 0.31 | −0.33 | 1.370 | 0.67 | −0.65 |
OC2 | −190.502 | 1.860 | 0.30 | −0.34 | 1.384 | 0.65 | −0.65 |
OC3 | −51.997 | 2.074 | - | −0.18 | 1.333 | 0.75 | −0.58 |
OS0 | −7.430 | - | - | −0.04 | 1.659 | 0.23 | −0.31 |
OS1 | −192.094 | 1.873 | 0.3 | −0.37 | 1.672 | 0.22 | −0.27 |
OS2 | −2.239 | - | - | −0.01 | 1.671 | 0.23 | −0.30 |
OS3 | −177.109 | 1.877 | 0.3 | −0.36 | 1.675 | 0.22 | −0.24 |
OS4 | 80.323 | - | - | 0.23 | 1.608 | 0.24 | −0.73 |
OH0 | −241.446 | 1.788 | 0.34 | −0.40 | 1.005 | 0.37 | −0.26 |
OH1 | −199.484 | 1.854 | 0.31 | −0.34 | - | - | −0.20 |
OH2 | −236.457 | 1.768 | 0.35 | −0.39 | 1.003 | 0.54 | −0.24 |
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Shi, Y.; Zhang, H.; Yu, J.; Feng, Y.; Jin, Y. Experimental and DFT Studies of Influence of Flue Gas Components on the Interaction between CaO and As during Sludge Combustion. Energies 2024, 17, 2522. https://doi.org/10.3390/en17112522
Shi Y, Zhang H, Yu J, Feng Y, Jin Y. Experimental and DFT Studies of Influence of Flue Gas Components on the Interaction between CaO and As during Sludge Combustion. Energies. 2024; 17(11):2522. https://doi.org/10.3390/en17112522
Chicago/Turabian StyleShi, Yilin, Huan Zhang, Jingxiang Yu, Youxiang Feng, and Yan Jin. 2024. "Experimental and DFT Studies of Influence of Flue Gas Components on the Interaction between CaO and As during Sludge Combustion" Energies 17, no. 11: 2522. https://doi.org/10.3390/en17112522
APA StyleShi, Y., Zhang, H., Yu, J., Feng, Y., & Jin, Y. (2024). Experimental and DFT Studies of Influence of Flue Gas Components on the Interaction between CaO and As during Sludge Combustion. Energies, 17(11), 2522. https://doi.org/10.3390/en17112522