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ACKNOWLEDGMENTS
We thank members of the Kadoch and Muir laboratories for
helpful advice and discussions throughout this project. We thank
N. Hananya, S. Daley, and F. Wojcik for providing peptide
materials.Funding:This work was supported by a Mark
Foundation for Cancer Research Emerging Leader Award (C.K.);
National Institutes of Health grant 1DP2CA195762-01 (C.K.);
a Pew-Stewart Scholars in Cancer Research Award (C.K.);
American Cancer Society Research Scholar Award RSG-14-051-
01-DMC (C.K.); National Institutes of Health grant R37-
GM086868 (T.W.M.); National Institutes of Health grant
PO1-CA196539 (T.W.M.); National Institutes of Health grant
K99/R00 K99CA237855 (N.M.); a Jane Coffin Childs Memorial
Fund Postdoctoral Fellowship Award (H.T.D.); and National
Institutes of Health grant GM123659 (J.D.B.).Author
contributions:Conceptualization: N.M., H.T.D., T.W.M., and
C.K. Methodology: N.M., H.T.D., T.W.M., and C.K. Investigation:
N.M., H.T.D., A.J.C., H.L., J.D.B., E.J.G., M.F., B.C.M., and
G.P.D. Data analysis, statistics, visualization: A.S., H.T.D., A.R.D.,
and J.D.B. Funding acquisition: T.W.M. and C.K. Supervision:
T.W.M. and C.K. Writing–original draft: N.M., H.T.D., T.W.M.,
and C.K. Writing–review & editing: N.M., H.T.D., T.W.M., and
C.K.Competing interests:C.K. is the scientific founder,
fiduciary board of directors member, scientific advisory boardmember, shareholder, and consultant for Foghorn Therapeutics,
Inc.(Cambridge,MA).T.W.M.isaninventoronUSpatent
10,087,485 held by Princeton University, which covers the
generation and use of DNA-barcoded nucleosome libraries. The
other authors declare that they have no competing interests.
Data and materials availability:All data are available in the
main text or the supplementary materials.SUPPLEMENTARY MATERIALS
science.sciencemag.org/content/373/6552/306/suppl/DC1
Materials and Methods
Figs. S1 to S4
Tables S1 to S3
References ( 42 , 43 )
MDAR Reproducibility Checklist
Data S1 to S1024 November 2020; accepted 4 June 2021
10.1126/science.abf8705GAS SEPARATION
Self-assembled iron-containing mordenite monolith
for carbon dioxide sieving
Yu Zhou^1 †, Jianlin Zhang^1 †, Lei Wang^2 †, Xili Cui3,4†, Xiaoling Liu^1 †, Sie Shing Wong5,6, Hua An5,6,
Ning Yan^5 , Jingyan Xie^1 , Cong Yu^3 , Peixin Zhang^3 , Yonghua Du7,8, Shibo Xi^7 , Lirong Zheng^9 ,
Xingzhong Cao^10 , Yajing Wu^2 , Yingxia Wang^11 , Chongqing Wang^1 , Haimeng Wen^1 , Lei Chen^1 ,
Huabin Xing3,4, Jun Wang^1 *
The development of low-cost, efficient physisorbents is essential for gas adsorption and separation; however,
the intrinsic tradeoff between capacity and selectivity, as well as the unavoidable shaping procedures of
conventional powder sorbents, greatly limits their practical separation efficiency. Herein, an exceedingly
stable iron-containing mordenite zeolite monolith with a pore system of precisely narrowed microchannels
was self-assembled using a one-pot template- and binder-free process. Iron-containing mordenite monoliths
that could be used directly for industrial application afforded record-high volumetric carbon dioxide uptakes
(293 and 219 cubic centimeters of carbon dioxide per cubic centimeter of material at 273 and 298 K,
respectively, at 1 bar pressure); excellent size-exclusive molecular sieving of carbon dioxide over argon,
nitrogen, and methane; stable recyclability; and good moisture resistance capability. Column breakthrough
experiments and process simulation further visualized the high separation efficiency.
P
hysical adsorption offers a promising
alternative to the established energy-
intensive processes in gas storage, sepa-
ration, and purification because of its
low energy consumption and mild ope-
rating conditions ( 1 – 6 ). One of the most pres-
sing issues in this field is the development of
low-cost and efficient physisorbents for CO 2
capture, including natural gas and biogas up-
grading (CO 2 /CH 4 separation), as well as CO 2
capture from postcombustion gases (CO 2 /N 2
separation) ( 6 – 11 ). However, the similar kinetic
diameters and physicochemical properties of
these gas molecules make the design of robust
physisorbents with simultaneously high uptake
and selectivity extremely challenging ( 6 , 8 , 12 ).
Enhanced selectivity is usually accompanied by
decreased adsorption capacity ( 5 , 8 ), which has
hindered the development of highly selective
CO 2 physisorbents with large uptakes. Conven-
tional syntheses produce sorbent materials as
powders that need to be postshaped, usually by
pressurizing or with the use of binders ( 4 , 13 ),
and the resultant pore blockage or collapse or
dilution of sorption sites inevitably decrease
sorption capacity and rate. Although self-shaped
physisorbents with large uptake, high selectiv-
ity, and fast adsorption-desorption kinetics
are preferable for industry, they present great
challenges for materials engineering.Ordered microporous materials are poten-
tial candidates for physisorbents with excellent
selectivity given their molecular sieving ability
( 3 , 6 , 9 – 16 ). Among them, zeolites (crystalline
aluminosilicates) are low cost and thermally
and hydrothermally stable and have been ap-
plied on large scales as catalysts and sorbents
( 13 – 17 ). The basic building units of zeolites are
rings with solidified members (8, 10, 12, and so
forth) mainly composed of Si, Al, and O atoms
( 10 , 14 , 17 , 18 ). Various approaches have been
proposed to improve the sorption performance
of zeolites by manipulating their topology,
morphology, and porosity ( 10 , 13 – 18 ). Nonethe-
less, precisely controlling zeolite pore aperture
within the kinetic diameters of gas molecules
involved in CO 2 capture (3 to 4 Å) is challeng-
ing ( 6 , 19 ). Although several self-shaped zeolites
have been constructed, they have unsatisfactory
mechanical strengths relative to those from tra-
ditional binder-aided postmolding technology
( 13 , 20 – 22 ).
We report a facile, template-free hydrother-
mal approach for self-assembling a hetero-
atomic zeolite monolith, Fe-containing
mordenite Fe-MOR(n) (wherenis the initial
Fe/Si molar ratio), which inherently has high
mechanical strength that could be directly
used as a shaped physisorbent. In CO 2 capture,
the Fe-MOR(n) series sieved CO 2 , Ar, N 2 , and
CH 4 in accordance with their molecular sizes
and exhibited unprecedented CO 2 uptakes and
CO 2 /Ar(N 2 , CH 4 ) selectivities with fast sorption
kinetics. The incorporation of isolated transi-
tion metal ions in the zeolite framework to
produce heteroatomic zeolites can add new
functionality ( 23 – 25 ). Generally, heteroatomic
zeolites have slightly larger pores because ofSCIENCEsciencemag.org 16 JULY 2021•VOL 373 ISSUE 6552 315
(^1) State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China. (^2) School of Chemistry and Molecular Engineering,
Nanjing Tech University, Nanjing 211816, China.^3 Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027,
China.^4 Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China.^5 Department of Chemical and Biomolecular Engineering, National University of Singapore,
Singapore 117585, Singapore.^6 Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China.^7 Institute of Chemical
and Engineering Sciences, Jurong Island, Singapore 627833, Singapore.^8 National Synchrotron Light Source II, Brookhaven National Lab, Upton, NY 11973, USA.^9 Beijing Synchrotron Radiation Facility, Institute of
High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.^10 Multi-discipline Research Division, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
*Corresponding author. Email: [email protected] (N.Y.); [email protected] (H.X.); [email protected] (J.W.)
†These authors contributed equally to this work.
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