Table2
典型载氮体介导的化学链合成氨过程
Nitrogen carrier | Nitrogen carrier type | Hydrogen source | Drive type | Reaction conditions | Reaction rate (efficiency) |
Ref. |
Ca3N2 | ionic nitride |
H2 | thermally driven |
N fixation:700 ℃ hydrogenation:550 ℃,1×105 Pa |
98 μmol/(g∙h) | [52] |
CrN | transition metal nitride | H2 | thermally driven |
N fixation:750 ℃ hydrogenation:700 ℃,1×105 Pa |
83.55 μmol/(g∙h) | [36] |
Co-CrN | transition metal nitride | H2 | thermally driven |
as above | 818.2 μmol/(g∙h) | [36] |
Mo2N | transition metal nitride | H2 | thermally driven |
N fixation:600 ℃ hydrogenation:450 ℃,1×105 Pa |
4576 μmol/(g∙h) | [32] |
BaNH | ionic nitride |
H2 | thermally driven |
N fixation & hydrogenation: 300 ℃,1×105 Pa |
198 μmol/(g∙h) | [66] |
Ni-baNH | ionic nitride |
H2 | thermally driven |
as above | 3125 μmol/(g∙h) | [66] |
Li2NH | ionic nitride |
H2 | thermoelectric coupling |
molten salt electrolytic cell: 2V,400 ℃,1×105 Pa |
64 μmol/(g∙h) | [71] |
Li3N | ionic nitride |
H2O | thermoelectric coupling |
electrolysis: 3V,450 ℃,1×105 Pa N fixation & hydrolysis: 100 ℃,1×105 Pa |
88.5% (initial current efficiency) |
[48] |
Mg3N2 | ionic nitride |
H2O | photothermal coupling |
N fixation:1×105 pa reduction & hydrolysis: <100 mTorr light source heating |
1.67 μmol/(g∙h) | [73] |
Mn5N2 | transition metal nitride | H2O | thermally driven |
hydrolysis: 500 ℃,1×105 Pa N fixation: 1150 ℃,1×105 Pa |
54%,2 h (the percentage of lattice nitrogen converted to ammonia) |
[77] |
CrN | transition metal nitride | H2O | thermally driven |
reduction: 1200−1500 ℃,1×105 Pa N fixation & hydrolysis: 1000 ℃,1×105 Pa |
108 μmol/(g∙h) | [78] |
AlN | covalent metal nitride | H2O | thermally driven |
N fixation: 1500−1700 ℃,1×105 pa hydrolysis: 1000 ℃,1×105 Pa |
88%,1 h (the percentage of lattice nitrogen converted to ammonia) |
[81] |
Table1
载氮体的常见制备方法
Method | Advantages | Disadvantages | Ref. |
Co-precipitation method |
the operation is simple, the cost is low, the prepared nitrogen carrier material has high hardness, uniform components, and dense powder | the addition of precipitant may lead to high local concentrations and agglomeration | [29] |
One-step pyrolysis method |
easy to operate, low preparation temperature and short time-consuming | the surface of the hydrogenated nitrogen carrier is rough and cracks appear | [30−33] |
Mechanical mixing method |
simple to operate and easy to control | poor uniformity and easy agglomeration | [34−35] |
Immersion method |
the operation is simple, easy to control, and the active component has a high atomic utilization | the preparation time is long, the uniformity is poor, and it is not suitable for industrial production | [34,36−37] |
Sol-gel method | the prepared sample has a high specific surface area, controllable microstructure and good uniformity | the cost of raw materials is high and the preparation time is long | [38] |
Molten salt synthesis method |
the operation is simple, the preparation temperature is low, the uniformity is good, and the product purity is high | the scope of application is small, the molten salt is toxic, and special equipment is required (PTFE lined steel reactor with nitrogen-filled glove box, etc.) | [39] |
Table3
反应1 h时不同焙烧温度n-Cr2O3催化正己烷脱氢反应
Sample | n-Cr2O3-600 | n-Cr2O3-700 | n-Cr2O3-800 | n-Cr2O3-950 |
Conversion of n-C6H14/% | 40.6 | 37.8 | 22.8 | 11.3 |
Selectivity to product/% | ||||
n-C6H12 | 20.1 | 21.5 | 25.1 | 28.2 |
C6H6 | 69.3 | 68.1 | 64.4 | 60.6 |
2,4-C6H10 | 2.9 | 3.0 | 3.1 | 3.2 |
Cracking products | 3.2 | 2.9 | 2.8 | 2.9 |
Isomerization products | 2.8 | 2.9 | 2.9 | 3.0 |
Others | 1.7 | 1.6 | 1.7 | 2.1 |
主办单位:煤炭科学研究总院有限公司 中国煤炭学会学术期刊工作委员会