化工学报 ›› 2021, Vol. 72 ›› Issue (9): 4469-4478.DOI: 10.11949/0438-1157.20210291
收稿日期:
2021-02-25
修回日期:
2021-05-17
出版日期:
2021-09-05
发布日期:
2021-09-05
通讯作者:
尹红
作者简介:
陈志荣(1963—),男,硕士,教授,Zhirong CHEN(),Yun TONG,Shenfeng YUAN,Hong YIN()
Received:
2021-02-25
Revised:
2021-05-17
Online:
2021-09-05
Published:
2021-09-05
Contact:
Hong YIN
摘要:
采用改变pH法在25、30和35℃下测定了质量浓度为0.25~4.0 mol/kg的KCl水溶液中蛋氨酸的解离常数,计算得到了蛋氨酸的质子化焓;采用电动势法在25℃测量了0.025~0.200 mol/kg蛋氨酸溶液中浓度为0.1~1 mol/kg的KCl的活度系数,计算得到了KCl溶液中蛋氨酸的活度系数。结果表明,蛋氨酸在KCl水溶液中的解离常数随温度上升而减小、随KCl浓度增加而增大;25℃下,蛋氨酸在KCl水溶液中的活度系数随蛋氨酸浓度增大先减小后增大。运用德拜-休克尔模型和Pitzer模型对解离常数和活度系数的实验数据进行拟合,得到了相关参数,结果表明Pitzer模型的可靠性较好。
中图分类号:
陈志荣, 童云, 袁慎峰, 尹红. 蛋氨酸在KCl溶液中的解离常数与活度系数[J]. 化工学报, 2021, 72(9): 4469-4478.
Zhirong CHEN, Yun TONG, Shenfeng YUAN, Hong YIN. Dissociation constants and activity coefficients of methionine in KCl aqueous solutions[J]. CIESC Journal, 2021, 72(9): 4469-4478.
T/℃ | mKCl/(mol/kg) | pK1* | pK2* | cKCl/(mol/L) | pK1* | pK2* |
---|---|---|---|---|---|---|
25 | 0.25 | 2.163±0.004 | 9.098±0.003 | 0.25 | 2.167 | 9.102 |
0.5 | 2.186±0.006 | 9.108±0.006 | 0.49 | 2.193 | 9.115 | |
1.0 | 2.240±0.003 | 9.138±0.004 | 0.97 | 2.254 | 9.152 | |
1.5 | 2.299±0.007 | 9.225±0.001 | 1.43 | 2.319 | 9.244 | |
2.0 | 2.361±0.009 | 9.300±0.006 | 1.89 | 2.387 | 9.326 | |
3.0 | 2.485±0.009 | 9.463±0.007 | 2.75 | 2.523 | 9.501 | |
4.0 | 2.616±0.010 | 9.640±0.007 | 3.55 | 2.667 | 9.691 | |
30 | 0.25 | 2.158±0.002 | 8.969±0.001 | 0.25 | 2.162 | 8.973 |
0.5 | 2.181±0.004 | 8.979±0.003 | 0.49 | 2.188 | 8.986 | |
1.0 | 2.230±0.002 | 9.028±0.004 | 0.97 | 2.243 | 9.041 | |
1.5 | 2.288±0.006 | 9.093±0.004 | 1.43 | 2.307 | 9.112 | |
2.0 | 2.344±0.005 | 9.167±0.008 | 1.89 | 2.370 | 9.193 | |
3.0 | 2.456±0.010 | 9.328±0.009 | 2.75 | 2.494 | 9.366 | |
4.0 | 2.587±0.011 | 9.500±0.012 | 3.55 | 2.640 | 9.551 | |
35 | 0.25 | 2.155±0.003 | 8.846±0.004 | 0.25 | 2.159 | 8.850 |
0.5 | 2.174±0.005 | 8.855±0.006 | 0.49 | 2.181 | 8.862 | |
1.0 | 2.223±0.002 | 8.903±0.005 | 0.97 | 2.236 | 8.916 | |
1.5 | 2.276±0.004 | 8.967±0.006 | 1.43 | 2.295 | 8.986 | |
2.0 | 2.330±0.006 | 9.038±0.005 | 1.89 | 2.356 | 9.064 | |
3.0 | 2.445±0.008 | 9.199±0.008 | 2.75 | 2.483 | 9.237 | |
4.0 | 2.564±0.010 | 9.369±0.011 | 3.55 | 2.615 | 9.420 |
表1 蛋氨酸在KCl水溶液中的解离常数
Table 1 pKi*(±S.D.) for methionine in KCl solutions at different temperatures
T/℃ | mKCl/(mol/kg) | pK1* | pK2* | cKCl/(mol/L) | pK1* | pK2* |
---|---|---|---|---|---|---|
25 | 0.25 | 2.163±0.004 | 9.098±0.003 | 0.25 | 2.167 | 9.102 |
0.5 | 2.186±0.006 | 9.108±0.006 | 0.49 | 2.193 | 9.115 | |
1.0 | 2.240±0.003 | 9.138±0.004 | 0.97 | 2.254 | 9.152 | |
1.5 | 2.299±0.007 | 9.225±0.001 | 1.43 | 2.319 | 9.244 | |
2.0 | 2.361±0.009 | 9.300±0.006 | 1.89 | 2.387 | 9.326 | |
3.0 | 2.485±0.009 | 9.463±0.007 | 2.75 | 2.523 | 9.501 | |
4.0 | 2.616±0.010 | 9.640±0.007 | 3.55 | 2.667 | 9.691 | |
30 | 0.25 | 2.158±0.002 | 8.969±0.001 | 0.25 | 2.162 | 8.973 |
0.5 | 2.181±0.004 | 8.979±0.003 | 0.49 | 2.188 | 8.986 | |
1.0 | 2.230±0.002 | 9.028±0.004 | 0.97 | 2.243 | 9.041 | |
1.5 | 2.288±0.006 | 9.093±0.004 | 1.43 | 2.307 | 9.112 | |
2.0 | 2.344±0.005 | 9.167±0.008 | 1.89 | 2.370 | 9.193 | |
3.0 | 2.456±0.010 | 9.328±0.009 | 2.75 | 2.494 | 9.366 | |
4.0 | 2.587±0.011 | 9.500±0.012 | 3.55 | 2.640 | 9.551 | |
35 | 0.25 | 2.155±0.003 | 8.846±0.004 | 0.25 | 2.159 | 8.850 |
0.5 | 2.174±0.005 | 8.855±0.006 | 0.49 | 2.181 | 8.862 | |
1.0 | 2.223±0.002 | 8.903±0.005 | 0.97 | 2.236 | 8.916 | |
1.5 | 2.276±0.004 | 8.967±0.006 | 1.43 | 2.295 | 8.986 | |
2.0 | 2.330±0.006 | 9.038±0.005 | 1.89 | 2.356 | 9.064 | |
3.0 | 2.445±0.008 | 9.199±0.008 | 2.75 | 2.483 | 9.237 | |
4.0 | 2.564±0.010 | 9.369±0.011 | 3.55 | 2.615 | 9.420 |
I/(mol/kg) | -ΔH1*/(kJ/mol) | -ΔH2*/(kJ/mol) |
---|---|---|
0.25 | 1.4 | 44.3 |
0.5 | 2.1 | 44.5 |
1.0 | 3.1 | 45.0 |
1.5 | 4.1 | 45.4 |
2.0 | 5.4 | 46.1 |
3.0 | 7.0 | 46.4 |
4.0 | 9.1 | 47.7 |
表2 蛋氨酸在不同离子强度下的质子化焓
Table 2 Enthalpy of dissolution at different ionic strength
I/(mol/kg) | -ΔH1*/(kJ/mol) | -ΔH2*/(kJ/mol) |
---|---|---|
0.25 | 1.4 | 44.3 |
0.5 | 2.1 | 44.5 |
1.0 | 3.1 | 45.0 |
1.5 | 4.1 | 45.4 |
2.0 | 5.4 | 46.1 |
3.0 | 7.0 | 46.4 |
4.0 | 9.1 | 47.7 |
mKCl/(mol/kg) | E+/mV | E-/mV | ΔE(1)/mV | ln(ms | |
---|---|---|---|---|---|
0.1 | 151.3 | 48.2 | 103.1 | 0.76777 | -2.5669 |
0.3 | 175.5 | 21.0 | 154.5 | 0.68627 | -1.5805 |
0.5 | 187.3 | 8.6 | 178.7 | 0.64902 | -1.1254 |
0.7 | 195.4 | 0.6 | 194.8 | 0.62599 | -0.8251 |
1.0 | 203.6 | -8.2 | 211.8 | 0.60389 | -0.5044 |
表3 电池(1)的电势值
Table 3 Values of electrochemical cell(1)
mKCl/(mol/kg) | E+/mV | E-/mV | ΔE(1)/mV | ln(ms | |
---|---|---|---|---|---|
0.1 | 151.3 | 48.2 | 103.1 | 0.76777 | -2.5669 |
0.3 | 175.5 | 21.0 | 154.5 | 0.68627 | -1.5805 |
0.5 | 187.3 | 8.6 | 178.7 | 0.64902 | -1.1254 |
0.7 | 195.4 | 0.6 | 194.8 | 0.62599 | -0.8251 |
1.0 | 203.6 | -8.2 | 211.8 | 0.60389 | -0.5044 |
mA/(mol/kg) | mKCl/(mol/kg) | ||||
---|---|---|---|---|---|
0.1 | 0.3 | 0.5 | 0.7 | 1.0 | |
0.025 | 1.0018 | 1.0022 | 1.0025 | 1.0029 | 1.0035 |
0.050 | 1.0026 | 1.0035 | 1.0041 | 1.005 | 1.0062 |
0.100 | 1.0026 | 1.0042 | 1.0058 | 1.0074 | 1.0099 |
0.150 | 1.0018 | 1.0045 | 1.0067 | 1.0093 | 1.0129 |
0.200 | 1.0019 | 1.0051 | 1.0082 | 1.0117 | 1.0165 |
表4 KCl在KCl-蛋氨酸水溶液和KCl溶液中的平均活度系数γ±(2)与γ±(1)的比值
Table 4 Ratio of mean ionic activity coefficient of KCl in methionine aqueous solution to that in water at different molalities of KCl and methionine
mA/(mol/kg) | mKCl/(mol/kg) | ||||
---|---|---|---|---|---|
0.1 | 0.3 | 0.5 | 0.7 | 1.0 | |
0.025 | 1.0018 | 1.0022 | 1.0025 | 1.0029 | 1.0035 |
0.050 | 1.0026 | 1.0035 | 1.0041 | 1.005 | 1.0062 |
0.100 | 1.0026 | 1.0042 | 1.0058 | 1.0074 | 1.0099 |
0.150 | 1.0018 | 1.0045 | 1.0067 | 1.0093 | 1.0129 |
0.200 | 1.0019 | 1.0051 | 1.0082 | 1.0117 | 1.0165 |
参数 | 参数值 |
---|---|
a1 | 1.5854×10-1 |
a2 | 1.5835×10-1 |
a3 | -1.6440 |
a4 | 6.6315×10-4 |
a5 | 4.3176 |
a6 | 1.3558×10-2 |
表5 式(29)参数值
Table 5 Coefficients of Eq.(29)
参数 | 参数值 |
---|---|
a1 | 1.5854×10-1 |
a2 | 1.5835×10-1 |
a3 | -1.6440 |
a4 | 6.6315×10-4 |
a5 | 4.3176 |
a6 | 1.3558×10-2 |
mA/(mol/kg) | mKCl/(mol/kg) | ||||
---|---|---|---|---|---|
0.1 | 0.3 | 0.5 | 0.7 | 1.0 | |
0.025 | 1.0093 | 1.0330 | 1.0641 | 1.1031 | 1.1784 |
0.050 | 1.0035 | 1.0153 | 1.0338 | 1.0595 | 1.1125 |
0.100 | 0.9967 | 0.9950 | 0.9998 | 1.0111 | 1.0408 |
0.150 | 0.9965 | 0.9944 | 0.9987 | 1.0097 | 1.0389 |
0.200 | 1.0027 | 1.0132 | 1.0305 | 1.0550 | 1.1064 |
表6 蛋氨酸在KCl-蛋氨酸水溶液与蛋氨酸水溶液中活度系数γA(2)和γA(1)的比值
Table 6 Ratio of mean ionic activity coefficients of methionine in the presence of KCl aqueous solution to that in water at different molalities of KCl and methionine
mA/(mol/kg) | mKCl/(mol/kg) | ||||
---|---|---|---|---|---|
0.1 | 0.3 | 0.5 | 0.7 | 1.0 | |
0.025 | 1.0093 | 1.0330 | 1.0641 | 1.1031 | 1.1784 |
0.050 | 1.0035 | 1.0153 | 1.0338 | 1.0595 | 1.1125 |
0.100 | 0.9967 | 0.9950 | 0.9998 | 1.0111 | 1.0408 |
0.150 | 0.9965 | 0.9944 | 0.9987 | 1.0097 | 1.0389 |
0.200 | 1.0027 | 1.0132 | 1.0305 | 1.0550 | 1.1064 |
i | Ai | S.E. | |
---|---|---|---|
1 | 0.2095 | 2.437 | 0.019 |
2 | 0.2380 | 9.339 | 0.0074 |
表7 DH模型参数
Table 7 Parameters of DH model
i | Ai | S.E. | |
---|---|---|---|
1 | 0.2095 | 2.437 | 0.019 |
2 | 0.2380 | 9.339 | 0.0074 |
T/K | Species | S.E. | ||||
---|---|---|---|---|---|---|
298.15 | H2B+ | -4.939 | 0.1009 | 9.316 | 0.03460 | 0.0019 |
303.15 | H2B+ | -4.912 | 0.1340 | 9.199 | 0.03002 | 0.0077 |
308.15 | H2B+ | -4.931 | 0.1040 | 9.348 | 0.0348 | 0.00169 |
298.15 | B- | -22.10 | 0.1530 | -5.810 | 0.05501 | 0.0110 |
303.15 | B- | -21.82 | 0.1594 | -5.807 | 0.05449 | 0.0125 |
308.15 | B- | -21.55 | 0.1593 | -5.771 | 0.05533 | 0.0128 |
表8 不同温度下KCl水溶液中蛋氨酸各形式的Pitzer模型参数
Table 8 Pitzer coefficients for methionine species in KCl media at different temperatures
T/K | Species | S.E. | ||||
---|---|---|---|---|---|---|
298.15 | H2B+ | -4.939 | 0.1009 | 9.316 | 0.03460 | 0.0019 |
303.15 | H2B+ | -4.912 | 0.1340 | 9.199 | 0.03002 | 0.0077 |
308.15 | H2B+ | -4.931 | 0.1040 | 9.348 | 0.0348 | 0.00169 |
298.15 | B- | -22.10 | 0.1530 | -5.810 | 0.05501 | 0.0110 |
303.15 | B- | -21.82 | 0.1594 | -5.807 | 0.05449 | 0.0125 |
308.15 | B- | -21.55 | 0.1593 | -5.771 | 0.05533 | 0.0128 |
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