Highly Efficient Synthesis of a Moisture-Stable Nitrogen-Abundant

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Highly efficient synthesis of a moisture-stable nitrogen-abundant MOF for large scale CO2 capture Chao Chen, Qingbin Jiang, Huifang Xu, and Zhan Lin Ind. Eng. Chem. Res., Just Accepted Manuscript • DOI: 10.1021/acs.iecr.8b05239 • Publication Date (Web): 17 Jan 2019 Downloaded from http://pubs.acs.org on January 19, 2019

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Industrial & Engineering Chemistry Research

Highly efficient synthesis of a moisture-stable nitrogenabundant MOF for large scale CO2 capture Chao Chen*, Qingbin Jiang, Huifang Xu, Zhan Lin* School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, Guangdong 510006, China KEYWORDS: microwave; nitrogen-abundant; metal organic framework; CO2 capture ABSTRACT:

Metal-organic frameworks (MOFs) hold great potential as CO2 adsorbents; however, long reaction time required for the preparation of MOFs by a hydrothermal or solvothermal method is a hurdle for large-scale production. In this work, we synthesize a moisture-stable nitrogenabundant cobalt-based MOF, i.e., Co-PL-1, by a microwave irradiation for the first time (denoted as MW-Co-PL-1). Compared to the hydrothermal synthesis that always takes 3 days at 180 oC, only 30 mins at the same temperature is required for the microwave synthesis. The resulting MW-Co-PL-1 shows high CO2 uptake, especially at low CO2 partial pressure (89 mg g-1 at 298 K, 1 bar and 53 mg g-1 at 298 K, 0.15 bar), good capture selectivity against N2 (19.8 at 1 bar and 44 at 0.15 bar), reversible CO2 uptake during consecutive adsorption-desorption cycles, and very robust structure stability in moisture conditions. The highly efficient synthesis together with great performance makes the microwave synthesis of Co-PL-1 promising for large-scale CO2 capture, which demonstrate a new way for large-scale application of MOFs in the near future.

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1. Introduction The increasing concentration of CO2 in the atmosphere has caused much public concern about climate change [1]. Anthropogenic CO2 emissions to the atmosphere are mainly due to the combustion of fossil fuels, which will still be the dominant energy resource in the foreseeable future [2]. In this context, carbon capture and storage (CCS) have been considered to be a promising strategy to alleviate CO2 emission problem in the short- to medium-term, as it can balance the utilization of fossil fuel energy and reduction of the CO2 emissions [3,4]. Among a variety of materials performing CCS, metal organic frameworks (MOFs) have been widely investigated owing to their several characteristics, such as large surface area, coordinatively unsaturated open metal sites, and surface functionalization [5-7]. Several classic MOFs, such as ZIFs [8], MOF-74 [9], HKUST-1 [10,11], MIL-101 [12,13], have been reported as excellent CO2 adsorbents. As well documented, MOFs will continue to be promising candidates as separation materials for CO2 capture. MOFs have been generally prepared through conventional hydrothermal or solvothermal synthesis. The major drawback of this method is long reaction time, which usually takes up to several days to form the product [14]. This limits large-scale application of MOFs, especially for CO2 capture from large-point sources that require huge amount of CO2 adsorbents. As such, developing new synthesis methods beyond the hydrothermal or solvothermal by using other energy sources have been widely studied, among which microwave energy has a special ability to affect materials syntheses. Compared to conventional hydrothermal or solvothermal synthesis, microwave synthesis has demonstrated the capability to increase energy efficiency and reduce reaction time over an order of magnitude. Several MOFs have been prepared through utilizing


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microwave energy, which definitely lower the cost to a large extent and make materials easily available for large-scale production [15,16]. In our previous study, we demonstrate that Co-PL-1 is an outstanding MOF material for CO2 capture [17]. The material is a three dimensional non-interpenetrated pillar-layered microporous MOF structure, in which the layers based on imidazole-4,5-dicarboxylic acid and the cobalt cluster are pillared by 4, 4’-bipyridyl (Fig. 1a and b). However, the preparation of Co-PL-1 by conventional hydrothermal synthesis takes 3 days. Thus, we intend to find a fast and controllable method to synthesize Co-PL-1 for their possible large-scale application. Herein, we utilize microwave as the energy source to successfully prepare Co-PL-1 in 30 mins (denoted as MWCo-PL-1). This is the first time this MOF material prepared by a microwave irradiation method. The MW-Co-PL-1 exhibits competitive attributes for CO2 capture, including high CO2 uptake (89 mg g-1 at 298 K, 1 bar and 53 mg g-1 at 298 K, 0.15 bar), good capture selectivity against N2 (19.8 at 1 bar and 44 at 0.15 bar), reversible CO2 capture during consecutive adsorptiondesorption cycles, and robust structure stability in moisture conditions. This work demonstrated that microwave synthesis is promising for large-scale production of Co-PL-1, which benefit its possible application for CO2 capture in the near future. 2. Preparation of Co-PL-1 by microwave irradiation 1.5 mmol Co(NO3)2∙6H2O was dissolved in 5 ml H2O to form a clear solution (1). In another batch, 1.5 mmol NaOH, 5 ml H2O, 1 mmol 4, 5-imidazole dicarboxylic acid, and 1 mmol 4, 4’-bipyridyl was mixed and stirred for 1 h to form a mixture (2). Solution 1 was added to mixture 2 to form the substrate mixture. The substrate mixture was transferred to a 35 ml capacity tube, sealed and heated to desired temperature under microwave irradiation. 160, 170, 180, 190, and 200 oC were studied as synthesis temperatures. 15, 30, 60, and 120 mins were


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studied as synthesis times. The product was named according to the synthesis temperature and time, for example, the product synthesized at 180 oC for 1 h was named as MW-180-1h.

3. Results and discussion 3.1. Characterization of materials In order to study the effect of synthesis time and temperature on the textural properties of resultant product, Co-PL-1 was prepared in a temperature range of 160 to 200 oC and a time range from 15 to 120 mins by microwave irradiation. The powder XRD patterns of Co-PL-1 samples obtained at different synthetic conditions were shown in Fig. 1c and d. The degree of Bragg diffraction angles of microwave synthesized Co-PL-1 (MW-Co-PL-1) were identical to those of hydrothermally synthesized Co-PL-1 (HT-Co-PL-1), confirming that the crystalline structure of Co-PL-1 was successfully obtained under microwave irradiation. However, the intensity of peaks was lower for MW-Co-PL-1 samples, indicating comparatively lower degree of crystallinity. The crystalline structure of Co-PL-1 can be formed in a wide range of temperatures (160-200 oC) with the time as short as 15 mins, indicating that Co-PL-1 can be effectively synthesized at different conditions.


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Figure 1. (a) A fragment of the Co-PL-1; (b) A single unit of coordinated molecular building blocks of Co-PL-1. Blue, red, and grey balls represent Cobalt, Oxygen, and Nitrogen atoms; (c) and (d) XRD patterns of Co-PL-1 prepared at different conditions; (e) N2 adsorption-desorption isotherms of Co-PL-1 samples. The textural properties of Co-PL-1 samples were characterized by N2 adsorption-desorption measurement. As shown in Fig. 1e, both the MW-Co-PL-1 and HT-Co-PL-1 exhibit type-I isotherms at low pressure range (P/P0 0.9) are ascribed to inter-particle voids between primary particles. The micropore volume of MW-Co-PL-1 (0.191 cm3 g-1) is smaller than that of HT-Co-PL-1 (0.277 cm3 g-1), demonstrating smaller microporosity of MW-Co-PL-1. On the meanwhile, the surface area of MW-Co-PL-1 (345 m2 g-1)


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is lower than 550 m2 g-1 of HT-Co-PL-1 (Table S1). These are due to comparatively lower degree of crystallinity of MW-Co-PL-1, which is consistent with XRD patterns in Fig. 1c and d.

Figure 2. SEM and TEM images of Co-PL-1 from (a), (c) hydrothermal synthesis and (b), (d) microwave synthesis. SEM and TEM images of the Co-PL-1 samples are shown in Fig. 2. Particles of MW-CoPL-1 are in uniform cubic shapes of about 100 nm diameter, whereas HT-Co-PL-1 is comprised of nanorod with particle length of about 350 nm. We believe that accelerated nucleation by microwave synthesis leads to smaller particles with different particle morphology. As shown in Fig. S1 and 2, there is no evident difference on the morphologies of MW-Co-PL-1 samples when synthesis temperature and time varies from 160 to 200 oC and 15 to 120 mins, respectively, indicating that the morphology of MW-Co-PL-1 was not severely affected by synthesis conditions.


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Based on the characterization results mentioned above, microwave irradiation at 180 oC for 30 mins is considered to be suitable to obtain Co-PL-1 with good quality. Further increasing temperature and time seems to have negligible effect on the textural properties of the material (Table 1). However, synthesis at lower temperature (160 or 170 oC) or shorter time (15 mins) leads to evident decrease of the surface area of Co-PL-1 (Table S1). The yield of MW-18030min is ca. 89.3%. 3.2. CO2 adsorption-desorption performance by MW-Co-PL-1 CO2 adsorption isotherms of MW-180-30min at 25 and 5 oC are shown in Fig. 3a. At 1 bar, the sample exhibits a CO2 uptake of 89 mg g-1 at 25 oC and 103 mg g-1 at 5 oC. This value is much lower than that achieved by HW-Co-PL-1 (128 mg g at 25 oC, Table 1). This is undoubtedly due to lower surface area of MW-Co-PL-1. In order to give a fair evaluation of the CO2 adsorption capacity of MW-180-30min, we list a series of reported CO2 adsorbents for comparison in Table 1. It can be clearly seen that the CO2 adsorption capacity of MW-18030min is comparable to most of reported CO2 adsorbents, including MOFs [16, 18-26], zeolites [27,28], carbons [29,30], and amine-functionalized silicas [31-33], indicating its competitive CO2 adsorption capability. In addition, rather than linear-type CO2 adsorption isotherm that usually exhibited by MOFs [8], MW-180-30min shows an arc-type CO2 adsorption isotherm. The CO2 adsorption capacity of MW-180-30min increased quickly at the low pressure range. For example, at 0.15 bar, the CO2 adsorption capacity reaches ca. 53 mg g-1, accounting for ca. 60% of the total capacity achieved at 1 bar. This indicates strong affinity of the material with CO2. We attribute this to abundant nitrogen atoms in two organic linkers (Fig. 1a and b), which can capture CO2 through strong quadrupolar interactions of carbon with nitrogen atom [25]. It is worth to mention that Lu et al. reported microwave synthesis of MOF-5 for CO2 capture [16].


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The microwave synthesized MOF-5 exhibited a CO2 adsorption capacity of 36 mg g-1 at 30 oC, 1 bar, which is much lower than CO2 uptake value achieved by MW-180-30min in our work.

Figure 3. (a) CO2 adsorption isotherm at 5 oC (square) and 25 oC (ball), and N2 adsorption isotherm at 25 oC (triangle) by MW-180-30min; (b) the isoteric heat of adsorption estimated as a function of the amount of CO2 adsorbed by MW-180-30min; (c) CO2 adsorption-desorption kinetics by MW-180-30min (adsorption at 25 oC); (d) CO2 adsorption-desorption recycle runs by MW-180-30min (adsorption at 25 oC and desorption at 65 oC).


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Table 1. A comparison of CO2 capture capacities of various reported CO2 adsorbents. Temperature

Pressure

CO2 uptake

(oC)

(bar)

(mg g-1)

MW-180-30min

25

1

89

Present work

MW-180-30min

5

1

103

Present work

HT-Co-PL-1

25

1

128

Present work

MOF-5

30

1

36

[16]

[Co2(tzpa)(μ3−OH)]

25

1

125

[18]

(Me2NH2) [In(SBA)2]

25

1

23

[19]

SNU-M10

25

1

92

[20]

Azo-UiO-66

25

1

34

[21]

SIFSIX-2-Cu-i

25

1

238

[22]

SodZMOF

25

1

60

[23]

[Ni(btzip)(H2btzip)]

25

1

209

[24]

ZIF-100

0

1

75

[25]

[Mn2(Hcbptz)2(Cl)]Cl

25

1

138

[26]

TiO2-modified 5A zeolite

25

0.5

71

[27]

ITQ-6-NH2

20

1

53

[28]

N-rich porous carbon

25

1

99

[29]

Amine-grafted porous carbon

25

1

50

[30]

SBA-15-NH2

0

1

78

[31]

PEI/SBA-15

45

1

80

[32]

MCM-48-NH2

25

0.15

70

[33]

Sample

Reference

The heat of CO2 adsorption is a useful indicator of the desorption energy, which is an important part of operational energy. We fitted experimental CO2 adsorption data of MW-18030min at 25 oC and 5 oC to the Langmuir-Freundlich equation, and calculated the material's heat


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of CO2 adsorption (Q) as a function of CO2 loading amount. As shown in Fig. 3b, the Q values (54-25 kJ mol-1) decreases with the CO2 loading, and were higher than literature values of several reported MOFs [11,23]. High values of Q indicate strong interaction between the adsorbent and CO2, which also explains why this material shows high CO2 uptake at low CO2 pressure range. High CO2 adsorption selectivity, especially against N2 gas, is necessary for post-combustion CO2 capture system, in which the flue gas contains a ca. 70% N2. N2 adsorption by MW-18030min at 25 oC was measured to check the CO2/N2 adsorption selectivity. As shown in Fig. 3a, the N2 uptake is only 4.5 mg g-1 at 1 bar. Based on the amounts of adsorbed gas at 1 bar, the CO2/N2 selectivity was calculated to be ca. 19.8. This value further increases to ca. 44 based on the adsorbed gas amount at 0.15 bar gas partial pressure. We also calculated the CO2/N2 adsorption selectivity for the mixture of CO2 and N2 gas in the ratio of 15:85 (Figure S3) by the Ideal Adsorbed Solution Theory (IAST). The CO2/N2 adsorption selectivity at 1 bar is 72.7, which is much higher compared to values exhibited by many reported MOFs under same conditions [26]. The high CO2 uptake at low CO2 partial pressure, together with high CO2/N2 adsorption selectivity, make MW-180-30min promising for post combustion CO2 capture, in which the CO2 concentration is below 15% with high concentration of N2 (ca. 70%) in the flue gas. The dynamic CO2 adsorption-desorption performance of MW-180-30min was also investigated. As shown in Fig. 3c. CO2 adsorption reaches the equilibrium within 15 mins, indicating a fast adsorption kinetics. This is very competitive as a CO2 adsorbent when compared to some reported CO2 adsorbents, such as amine-silica composites, which needs more than 1 h to reach its adsorption equilibrium. The open pore structure and large pore size (larger than the


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kinetic diameter of CO2) of MW-180-30min facilitates the CO2 diffusion inside the pore structure and enable CO2 reach the CO2-affinity sites easily. Temperature and pressure swing were both conducted to study the suitable condition for adsorbent regeneration. As shown in Fig. 3c, when the adsorbent was treated at 35 oC with Ar purge, only 68 % of CO2 can be desorbed in 50 mins. This result shows the strong affinity of MW-180-30min with CO2, which is also consistent with its high CO2 adsorption heat. 50 oC is enough to desorb all captured CO2 in 50 min, while further increasing desorption temperature leads to faster CO2 desorption rate. The cyclic performance of the MW-180-30min was studied by conducting consecutive CO2 adsorption-desorption runs. The adsorption and desorption temperature were set at 35 and 65 oC, respectively. As shown in Fig. 3d, the material shows very stable CO2 adsorption-desorption performance in 10 runs without the reduction of CO2 adsorption capacity. Moreover, stability in moisture conditions is quite important for MOF materials for their practical application. For example, MOF-5 has been investigated in various fields, such as gas storage and separation, as well as in catalysis [34]. However, MOF-5 is unstable in moisture, which hinders its progress for practical application. MW-180-30min can be synthesized in water at temperature as high as 180 oC

under autogenous pressure, demonstrating that its structure is robust in moisture condition.

This makes MW-180-30min quite promising for practical applications. 4. Conclusion To sum up, we synthesize a moisture-stable nitrogen-abundant MOF, Co-PL-1, by microwave irradiation method for the first time. The synthesis time is remarkably reduced to 30 min from 3 days for hydrothermal synthesis. Microwave synthesized Co-PL-1 exhibits competitive attributes for CO2 capture, including high CO2 adsorption capacity and selectivity against N2, reversible cyclic CO2 adsorption-desorption, and exceptional stability in moisture.


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The great reduction of synthesis time, together with outstanding properties of MW-Co-PL-1 as a CO2 adsorbent, make the microwave synthesis method promising for large-scale production of Co-PL-1 for CO2 capture in the near future. AUTHOR INFORMATION Corresponding Authors *Email address: [email protected]; [email protected] ACKNOWLEDGMENT This work was financially supported by the National Natural Science Foundation of China (No. 21607121). Supporting Information Available: Experimental details, such as material synthesis and characterization; CO2 or N2 adsorption-desorption measurements; SEM images of Co-PL-1 from microwave synthesis at different conditions; Textural properties of microwave synthesized CoPL-1 samples. REFERENCES [1] Stern, N. Review on the Economics of Climate Change. Cambridge University Press, Cambridge, 2006. [2] Rackley, S. A. Carbon Capture and Storage. Elsevier, 2010. [3] Figueroa, J. D.; Fout, T.; Plasynski, S.; McIlvried, H.; Srivastava, R. D. Advances in CO2 capture technology—The U.S. department of energy’s carbon sequestration program. Int. J. Greenhouse Gas control. 2008, 2, 9-20.


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A moisture-stable nitrogen-abundant MOF, Co-PL-1, was firstly synthesized in 30 min by microwave irradiation. The resultant material shows high CO2 uptake, especially at low CO2 partial pressure, good capture selectivity against N2, reversible CO2 uptake during consecutive adsorption-desorption cycles, and very robust structure stability in harsh conditions.


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Highly Efficient Synthesis of a Moisture-Stable Nitrogen-Abundant

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