Electronic Supplementary Information deficient” phase ... · Partial acetylene hydrogenation was performed in a consecutive fixed-bed reactor equipped with a quartz reaction tube
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Electronic Supplementary Information
Outstanding catalytic performance of semi-hydrogenation of
acetylene under front-end process by establishing “hydrogen
Table S1 Summarized results of publications in acetylene hydrogenation
Reaction Results Catalyst Reaction Condition
This
work
XC2H2=99.5%
SC2H4=91%0.03%Pd-[Bmim][Cl]/ Al2O3
T=120 ℃, P=0.1 MPaGHSV= 6000 h -1
Hydrogen : Acetylene mole ratio=20:1
1[2]XC2H2=98%
SC2H4=80%1 wt% Pd/SiC
T=65℃, P=0.1MPaSpace velocity =30,000 ml min-1 g-1
Hydrogen : Acetylene mole ratio≈2:1
2[3]XC2H2=80%
SC2H4=80%0.005%Pd/Ni(OH)2
T=105℃,Flow rate=40 ml min-1
The reactant gas mixture
(0.65vol% acetylene, 5vol% hydrogen, and 50.5vol%
ethylene balanced with argon)
3[4]XC2H2=99%
SC2H4=83%
0.5wt% single-atom
Pd1/C3N4
T=115℃space velocity = 60000 mL·g-1·h-1
pressure = 0.1 MPa.
hydrogen : acetylene mole ratio=2:1
4[5]XC2H2>99%
SC2H4=70-80%Pd/COP
T=120℃space velocity =0.02 molC2H2molPd
-1·s1
Gas mixture: 0.6 kPa C2H2, 0.6 kPa C3H8, 49.3 kPa
C2H4, 0.9 kPaH2 and 48.6 kPa N2
5[6]XC2H2>99%
SC2H4=83.8%PdAg/Mg0.5Ti0.5Oy
T=70℃,P=0.4MPaspace velocity (GHSV) =10050 h-1
hydrogen : acetylene ratio=2:1
6[7]XC2H2=85.9%
SC2H4=87.2%Pd-Ga/MgO-Al2O3
T=45℃,P=0.05MPaspace velocity (GHSV) =10056 h-1
hydrogen : acetylene ratio=2:1
7[8]XC2H2=96%
SC2H4≈90%0.01%Pd/LSA-SiO2
T=100℃space velocity (GHSV)=3600ml gcat.
-1h-1
hydrogen : acetylene ratio=6:1
8[9]XC2H2=100%
SC2H4≈85%CuPd0.006/SiO2
T=160℃gas velocity=240000ml h-1 g-1
hydrogen : acetylene ratio=20:1
9[10]XC2H2=96%
SC2H4=92%PdIn/MgAl2O4
T=90℃space velocity (GHSV)=288000ml h-1 g-1
hydrogen : acetylene ratio=10:1
10[11]XC2H2=95%
SC2H4=80%InPd2
T=200℃Flow=30 cm3 min-1
hydrogen : acetylene ratio=10:1
11[12]XC2H2=100%
SC2H4=83%Pd4S/CNF
T=250℃space velocity (GHSV)=60000ml h-1 g-1
12[13]XC2H2=100%
SC2H4=82%
Mco-PdCu/MgAl-
cHTnanoalloy catalyst
T=100℃,P=0.4MPaspace velocity (GHSV) =10050 h-1
hydrogen : acetylene ratio=2:1
4. Solubility measurement
Fig. S7 presents the schematic diagram of the experimental apparatus, which is
similar to previous publication[14]. It mainly consists of a 316-L stainless steel reactor
with a magnetic stirrer(39.8 mL), a gas reservoir(500 mL), a vacuum pump, a water
bath, and two pressure sensors (Rosemount 3051) with an accuracy of 0.03 kPa in the
experimental pressure range.
For each experimental run, about 8 g ionic liquid was placed in the reactor. The
reactor was closed and kept under vacuum (1 kPa) at the 100 ℃ to degas the
absorbent as well as to test the gas leak. Then a certain amount of gas was introduced
to the gas reservoir supplied by the gas cylinder. The inlet gas valve was open until
the pressure reached the about 103 kPa. To ensure that the temperature equilibrium
had been reached, both reactor and reservoir were placed in oil bath for about 1 h, and
the original pressure/temperature was recorded. The equilibrium process begins with
opening the gas inlet valve (the valve should be closed immediately) to make the gas
transfer from gas reservoir to reactor. Finally, when the pressure of reactor was
constant, the soluble equilibrium was arrived and the pressure/temperature of
reservoir and reactor was recorded. Therefore, the solubility of gas can be calculated
and the formulas were as follows:
(3-1)𝑉𝑅𝑎= 𝑉𝑅 ‒ 𝑚𝐼𝐿 × 𝜌𝐼𝐿
(3-2) 1
a11
R
RRR TR
VPn
(3-3)2
a22
R
RRR TR
VPn
(3-4)
1
11
S
SSS TR
VPn
(3-5)2
22
S
SSS TR
VPn
(3-6)IL
RRSS
mnnnnS )()( 1221
VRa: Actual volume of reactor
VR: Original volume of reactor
VS: Volume of reservoir
PR1: Pressure of reactor before adsorption
PS1: Pressure of reservoir before adsorption
PR2: Pressure of reactor when the adsorption is balanced
PS2: Pressure of reservoir when the adsorption is balanced
TR1: Temperature of reactor before adsorption
TR2: Temperature of reactor when the adsorption is balanced
TS1: Pressure of reservoir before adsorption
TS2: Pressure of reservoir when the adsorption is balanced
nR1: Mole amount of gas in reactor before adsorption
nR2: Mole amount of gas in reactor when the adsorption is balanced
nS1: Mole amount of gas in reservoir before adsorption
nS2: Mole amount of gas in reservoir when the adsorption is balanced
mIL: Mass of ionic liquid
ρIL: Density of ionic liquid
S: Solubility of gas
Fig. S8 The set-up for measuring the gas solubility
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