Chemical Industry and Engineering Progress ›› 2023, Vol. 42 ›› Issue (2): 783-793.DOI: 10.16085/j.issn.1000-6613.2022-0630
• Industrial catalysis • Previous Articles Next Articles
LI Naizhen1(), SUN Ruijie1, QIN Zhifeng1,2,3(), MIAO Maoqian1, WU Qiongxiao4, CHANG Liping1, SUN Pengcheng2, ZENG Jian2, LIU Yi3
Received:
2022-04-12
Revised:
2022-06-19
Online:
2023-03-13
Published:
2023-02-25
Contact:
QIN Zhifeng
李乃珍1(), 孙瑞洁1, 秦志峰1,2,3(), 苗茂谦1, 吴琼笑4, 常丽萍1, 孙鹏程2, 曾剑2, 刘毅3
通讯作者:
秦志峰
作者简介:
李乃珍(1995—),女,硕士研究生,研究方向为气体净化与工业催化。E-mail:lnzlldmmmmd@163.com。
基金资助:
CLC Number:
LI Naizhen, SUN Ruijie, QIN Zhifeng, MIAO Maoqian, WU Qiongxiao, CHANG Liping, SUN Pengcheng, ZENG Jian, LIU Yi. Effects of constant carbon atmosphere on the activity, selectivity and coking of catalysts in hydrodesulfurization of coke oven gas[J]. Chemical Industry and Engineering Progress, 2023, 42(2): 783-793.
李乃珍, 孙瑞洁, 秦志峰, 苗茂谦, 吴琼笑, 常丽萍, 孙鹏程, 曾剑, 刘毅. 焦炉煤气常量含碳气氛对加氢脱硫催化剂活性、选择性和积炭的影响[J]. 化工进展, 2023, 42(2): 783-793.
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气体名称 | 纯度(体积分数)或含量 | 平衡气体 |
---|---|---|
甲烷 | 99.99% | — |
乙烯 | 99.9% | — |
乙烷 | 99.9% | — |
一氧化碳 | 99.99% | — |
二氧化碳 | 99.99% | — |
预硫化气体 | H2S约3% | H2 |
含硫反应气体 | COS约119.48mg/m3、CS2约91.28mg/m3、C4H4S约12.39mg/m3 | H2 |
TPRS反应气1 | COS约2080mg/m3 | H2 |
TPRS反应气2 | H2S约500mg/m3 | H2 |
硫化物标气 | H2S约143.32mg/m3、COS约155.40mg/m3、CH3SH约99.35mg/m3、C2H5SH约98.54mg/m3、CH3SCH3约102.23mg/m3、CS2约157.02mg/m3、C4H4S约147.57mg/m3、CH3S2CH3约148.57mg/m3、C2H5SCH3约146.79mg/m3、(C2H5)S约146.45mg/m3 | N2 |
气体名称 | 纯度(体积分数)或含量 | 平衡气体 |
---|---|---|
甲烷 | 99.99% | — |
乙烯 | 99.9% | — |
乙烷 | 99.9% | — |
一氧化碳 | 99.99% | — |
二氧化碳 | 99.99% | — |
预硫化气体 | H2S约3% | H2 |
含硫反应气体 | COS约119.48mg/m3、CS2约91.28mg/m3、C4H4S约12.39mg/m3 | H2 |
TPRS反应气1 | COS约2080mg/m3 | H2 |
TPRS反应气2 | H2S约500mg/m3 | H2 |
硫化物标气 | H2S约143.32mg/m3、COS约155.40mg/m3、CH3SH约99.35mg/m3、C2H5SH约98.54mg/m3、CH3SCH3约102.23mg/m3、CS2约157.02mg/m3、C4H4S约147.57mg/m3、CH3S2CH3约148.57mg/m3、C2H5SCH3约146.79mg/m3、(C2H5)S约146.45mg/m3 | N2 |
序号 | 反应方程式 | ΔG/kJ·mol-1 | lgK | ||
---|---|---|---|---|---|
250℃ | 350℃ | 250℃ | 350℃ | ||
(1) | COS+H2=CO+H2S | -2.444 | -3.277 | 1.021 | 1.149 |
(2) | COS+4H2=H2S+CH4+H2O | -20.480 | -13.451 | 8.556 | 4.718 |
(3) | COS+H2O=CO2+H2S | -10.755 | -12.811 | 4.493 | 4.493 |
(4) | 2COS+4H2=CH4+CS2+2H2O | -13.972 | -8.843 | 5.837 | 3.102 |
(5) | CS2+4H2=2H2S+CH4 | -34.279 | -29.596 | 14.322 | 10.381 |
(6) | C4H4S+4H2=H2S+i-C4H10 | -25.936 | -17.916 | 10.836 | 6.284 |
(7) | CO2+CS2=2COS | -3.044 | -3.335 | 1.272 | 1.170 |
(8) | CO2+H2=CH4+2H2O | -17.016 | -12.178 | 7.109 | 4.271 |
(9) | H2S+CO=COS+H2+CH4 | -14.350 | -6.113 | 5.996 | -1.999 |
(10) | H2+CO=CO2+CH4 | -26.348 | -19.708 | 11.008 | 6.912 |
(11) | COS+3H2=CH3SH+H2O | -2.893 | 4.073 | 1.209 | -1.429 |
(12) | CS2+3H2=CH3SH+H2S | -16.692 | -12.072 | 6.974 | 4.234 |
(13) | 2CH3SH=(CH3)2S+H2S | -0.146 | 0.284 | 0.061 | -0.100 |
(14) | CH3SH+H2=CH4+H2S | -17.587 | -17.524 | 7.348 | 6.147 |
(15) | (CH3)2S+2H2=2CH4+H2S | -35.028 | -35.332 | 14.634 | 12.393 |
(16) | C2H4+H2S=C2H5SH | -2.850 | 0.202 | 1.191 | -0.071 |
(17) | 2C2H5SH=(C2H5)2S+H2S | -1.122 | -0.968 | 0.469 | 0.340 |
(18) | C2H5SH+C2H4=(C2H5)2S | -3.972 | -0.767 | 1.660 | 0.269 |
(19) | C2H4+CH3SH=CH3SC2H5 | -3.373 | -0.021 | 1.409 | 0.007 |
(20) | C2H5SH+H2=C2H6+H2S | -14.574 | -14.504 | 6.089 | 5.087 |
(21) | CO+3H2=CH4+H2O | -18.036 | -10.174 | 7.535 | 3.569 |
(22) | CO+H2O=CO2+H2 | -8.312 | -9.534 | 3.473 | 3.344 |
序号 | 反应方程式 | ΔG/kJ·mol-1 | lgK | ||
---|---|---|---|---|---|
250℃ | 350℃ | 250℃ | 350℃ | ||
(1) | COS+H2=CO+H2S | -2.444 | -3.277 | 1.021 | 1.149 |
(2) | COS+4H2=H2S+CH4+H2O | -20.480 | -13.451 | 8.556 | 4.718 |
(3) | COS+H2O=CO2+H2S | -10.755 | -12.811 | 4.493 | 4.493 |
(4) | 2COS+4H2=CH4+CS2+2H2O | -13.972 | -8.843 | 5.837 | 3.102 |
(5) | CS2+4H2=2H2S+CH4 | -34.279 | -29.596 | 14.322 | 10.381 |
(6) | C4H4S+4H2=H2S+i-C4H10 | -25.936 | -17.916 | 10.836 | 6.284 |
(7) | CO2+CS2=2COS | -3.044 | -3.335 | 1.272 | 1.170 |
(8) | CO2+H2=CH4+2H2O | -17.016 | -12.178 | 7.109 | 4.271 |
(9) | H2S+CO=COS+H2+CH4 | -14.350 | -6.113 | 5.996 | -1.999 |
(10) | H2+CO=CO2+CH4 | -26.348 | -19.708 | 11.008 | 6.912 |
(11) | COS+3H2=CH3SH+H2O | -2.893 | 4.073 | 1.209 | -1.429 |
(12) | CS2+3H2=CH3SH+H2S | -16.692 | -12.072 | 6.974 | 4.234 |
(13) | 2CH3SH=(CH3)2S+H2S | -0.146 | 0.284 | 0.061 | -0.100 |
(14) | CH3SH+H2=CH4+H2S | -17.587 | -17.524 | 7.348 | 6.147 |
(15) | (CH3)2S+2H2=2CH4+H2S | -35.028 | -35.332 | 14.634 | 12.393 |
(16) | C2H4+H2S=C2H5SH | -2.850 | 0.202 | 1.191 | -0.071 |
(17) | 2C2H5SH=(C2H5)2S+H2S | -1.122 | -0.968 | 0.469 | 0.340 |
(18) | C2H5SH+C2H4=(C2H5)2S | -3.972 | -0.767 | 1.660 | 0.269 |
(19) | C2H4+CH3SH=CH3SC2H5 | -3.373 | -0.021 | 1.409 | 0.007 |
(20) | C2H5SH+H2=C2H6+H2S | -14.574 | -14.504 | 6.089 | 5.087 |
(21) | CO+3H2=CH4+H2O | -18.036 | -10.174 | 7.535 | 3.569 |
(22) | CO+H2O=CO2+H2 | -8.312 | -9.534 | 3.473 | 3.344 |
样品 | 孔体积/cm3·g-1 | 比表面积/m2·g-1 | 平均孔径/nm | 碳质量分数/% | 硫质量分数/% |
---|---|---|---|---|---|
新鲜催化剂 | 0.47 | 210.4 | 4.4 | 0.12 | 0.12 |
硫化后催化剂 | 0.45 | 190.8 | 4.4 | 0.29 | 3.62 |
N2反应后 | 0.43 | 185.6 | 4.5 | 0.38 | 2.48 |
CH4反应后 | 0.41 | 181.9 | 4.5 | 0.44 | 2.64 |
C2H4反应后 | 0.41 | 178.1 | 4.6 | 0.77 | 2.56 |
C2H6反应后 | 0.41 | 181.4 | 4.5 | 0.29 | 2.72 |
CO反应后 | 0.42 | 182.5 | 4.5 | 0.47 | 2.56 |
CO2反应后 | 0.42 | 184.4 | 4.5 | 0.54 | 2.58 |
样品 | 孔体积/cm3·g-1 | 比表面积/m2·g-1 | 平均孔径/nm | 碳质量分数/% | 硫质量分数/% |
---|---|---|---|---|---|
新鲜催化剂 | 0.47 | 210.4 | 4.4 | 0.12 | 0.12 |
硫化后催化剂 | 0.45 | 190.8 | 4.4 | 0.29 | 3.62 |
N2反应后 | 0.43 | 185.6 | 4.5 | 0.38 | 2.48 |
CH4反应后 | 0.41 | 181.9 | 4.5 | 0.44 | 2.64 |
C2H4反应后 | 0.41 | 178.1 | 4.6 | 0.77 | 2.56 |
C2H6反应后 | 0.41 | 181.4 | 4.5 | 0.29 | 2.72 |
CO反应后 | 0.42 | 182.5 | 4.5 | 0.47 | 2.56 |
CO2反应后 | 0.42 | 184.4 | 4.5 | 0.54 | 2.58 |
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