Metal-organic frameworks (MOFs) have great potentials as adsorbents for natural gas purification. However

the trade-off between selectivity and adsorption capacity remains a challenge. Herein

we report a pillared-layer metal-organic framework Ni(HBTC)(bipy) for efficiently separating the C

3

H

8

/C

2

H

6

/CH

4

mixture. The experimental results show that the adsorption capacity of C

3

H

8

and C

2

H

6

on Ni(HBTC)(bipy) are as high as 6.18 and 5.85 mmol·g

-1

while only 0.93 mmol·g

-1

for CH

4

at 298 K and 100 kPa. Especially

the adsorption capacity of C

3

H

8

at 5 kPa can reach an unprecedented 4.52 mmol·g

-1

and for C

2

H

6

it is 1.48 mmol·g

-1

at 10 kPa. The ideal adsorbed solution theory predicted C

3

H

8

/CH

4

selectivity is as high as 1857.0

superior to most of the reported materials. Breakthrough experiment results indicated that material could completely separate the

C

3

H

8

/C

2

H

6

/CH

4

mixture. Therefore

Ni(HBTC)(bipy) is a promising material for separation of natural gas.