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436
CHEMICAL PROBLEMS 2020 no. 4 (18) ISSN 2221-8688
UDC 544.478-03
HYDROGEN-RICH GAS PRODUCTION BY CATALYTIC DECOMPOSITION OF OXYGENATED COMPOUNDS OF C1 CHEMISTRY
S.D. Badmaev1'2, A.E. Pinigina1'2, V.D. Belyaev 1, V.A. Sobyanin1
lBoreskov Institute of Catalysis, Prospekt Lavrentieva, 5, Novosibirsk, 630090 Russia 2Novosibirsk State University, Pirogova Str. 2, Novosibirsk, 630090, Russia e-mail: [email protected]
Received 02.10.2020 Accepted 13.12.2020
Abstract: Catalytic decomposition of oxygenated compounds of C1 chemistry into hydrogen rich gas was studied over Pt/CeO2-ZrO2 catalyst. In particular, formic acid, methanol, dimethyl ether and dimethoxymethane were decomposed under atmospheric pressure into hydrogen-rich gas at temperatures below 450 o C. Challenges and benefits of each reaction in producing hydrogen-rich gas for fuel cell feeding are discussed.
Key words: Catalytic decomposition, oxygenates, C1 chemistry, formic acid, methanol, dimethyl ether, dimethoxymethane, platinum, hydrogen, synthesis gas DOI: 10.32737/2221-8688-2020-4-436-444
1. Introduction
Ever-increasing role of modern electronic devices in the human life stimulates active research and development in low-power fuel cell based portable and autonomous power units [1, 2]. The fuel for such power units is hydrogen or hydrogen-rich gas, which can be produced by reforming hydrocarbons or oxygenates [3-6]. A literature survey of current studies shows that oxygenated compounds of C1 chemistry, such as formic acid (FA) [7-9], methanol [10, 11], dimethyl ether (DME) [12,13] and dimethoxymethane (DMM) [14-17], can be easily converted into hydrogen-rich gas at relatively low temperatures as compared to conventional hydrocarbon fuels. In addition, these oxygenates, unlike hydrocarbon fuels are free of impurities such as sulfur compounds that is a poison for most metal catalysts. The last
evidence means that no sulfur scrubbing reactor is required. Among the known processes for hydrocarbon catalytic conversion (steam reforming, partial oxidation and decomposition), decomposition is thought to be promising for creating a compact "fuel processor:" this process requires no water or air tanks and respective supply and flow control systems.
Based on the above facts and taking into account a good performance of Pt-containing catalyst in the decomposition of FA (1) [7], methanol (2) [10], DME (3) [12] and DMM (4) [15], as well as a lower cost of Pt as compared to Pd and Rh, we decided to perform comparative studies of catalytic decomposition of the mentioned oxygenated compounds into hydrogen rich gas over the Pt/CeO2-ZrO2 catalyst.
Overall FA and methanol decomposition reactions are expressed by equations as follows:
HCOOH = H2 + CO2 CH3OH = 2H2 + CO
(1) (2)
Overall DME and DMM decomposition reactions are most likely described by equations:
CH3OCH3 = H2 + CO + CH4 (3)
CHEMICAL PROBLEMS 2020 no. 4 (18)
www.chemprob.org
CH3OCH2OCH3 = 2H2 + 2CO + CH4 (4)
Purpose of the manuscript
The present work reports on the comparative analysis to elucidate the challenges
performance of the Pt/CeO2-ZrO2 catalyst in FA, and benefits of each reaction for producing
methanol, DME and DMM decomposition hydrogen-rich gas for fuel cell feeding. reactions into hydrogen-rich gas and provides a
2. Experimental procedure
Pt/CeO2-ZrO2 catalyst (1.9 wt % Pt) was prepared by sorption-hydrolytic deposition as described in [17,18]. A solution of H2PtCl4 was mixed with Na2CO3 providing the molar ratio of Na/Cl=1. The obtained mixture was brought into contact with an aqueous suspension of the CeO2-ZrO2 powder (Ecoalliance Ltd. Russia). According to our previous work [18], CeO2-ZrO2 support had fluorite structure with crystallite particles of 10 nm in size; the size of Pt particles in the fresh catalyst was ~2 nm. The BET specific surface area of Pt/CeO2-ZrO2 was ~70 m/g.
Catalytic experiments on FA, methanol, DME and DMM decomposition were performed in a U-shaped quartz reactor (i.d. 6 mm) under atmospheric pressure. Prior to the catalyst testing, the Pt/CeO2-ZrO2 catalyst (0.25-0.5 mm) was reduced in situ at 400 °C for 1 h using 10 vol. % H2/Ar with a total flow rate of 3000 mL/h.
C0 - C, x
X (%) =
C
W,
H
V Scat ' h J
Then the catalyst was exposed to the feed composed of (vol. %): 10 HCOOH and 90 N2 for FA decomposition; 10 CH3OH and 90 N2 for methanol decomposition; 10 CH3OCH2OCH3 and 90 N2 for DMM decomposition; 10 CH3OCH3 and 90 N2 for DME decomposition. Total gas hourly space velocity (GHSV) was 10000 h-1.
FA, methanol and DMM were introduced to the reactor by bubbling N2 through a saturator filled with respective liquid compound. Bronkhorst mass flow controllers fed the DME, N2 and H2 (for catalyst reduction). The composition of the reagents and reaction products were evaluated by a gas chromatograph (GC Chromos-1000). The FA, methanol, DME and DMM conversions (Xi) and H2 productivity (W(H2)) were calculated using the following equations:
C
N
C
x 100
F ■ C
r L ^ F Ch2
C0
CN2
C
^ AT
100-m„
(5)
(6)
0
where C, , C° are the inlet concentrations
(vol.%) of oxygenate (FA, methanol, DME and DMM) and N2;
C , C , C are the outlet concentrations
, 3 N 2 H2
(vol.%) of unconverted oxygenate, N2, H2. F - total flow rate of the inlet reaction mixture (L/h); mcat - catalyst weight (g).
The H2 selectivity (S(H2)) for decomposition reactions was calculated as total moles of H2 actually produced through division by the moles of H2 theoretically produced. The carbonaceous product selectivity (S) was defined as the amount of carbon in this product
divided by total amount of carbon in converted compound of C1 chemistry.
To evaluate carbon formation in DMM and DME decomposition, the spent catalysts were studied by temperature-programmed oxidation (TPO) using a TG209F Libra Termo microbalance instrument (Netzch, Germany). The feed gas, 6 vol.% O2/He, flowed at 4.2 L/h. The sample (~50 mg) was heated from 25 to 600 oC at 600 oC/h. The outlet CO2 concentration was monitored on-line by a QMS-200 mass-spectrometer (Stanford Research Systems, USA). The amount of the coke
deposited on the catalyst was determined from that of CO2 released in the TPO runs.
3. Results and discussion
3.1. Catalytic decomposition of formic acid
Fig. 1 shows the effect of temperature on FA conversion and product selectivity (H2, CO2, CO and CH4) in FA decomposition over Pt/CeO2-ZrO2 catalyst. As the reaction temperature increased from 150 to 400 °C, the FA conversion increased and reached ~100 % at ~200 °C. Hydrogen and carbon dioxide were the main reaction products (S > 80 %), suggesting that the FA decomposition
predominantly proceeds according to equation (1). Note that the temperature dependencies of H2 and CO2 selectivities were similar: the maximum in both curves (~94 %) was observed at temperatures of 250-300 °C. Further decrease of the selectivities at temperatures above 300 °C is explained by intensification of side reactions (7) and (8) yielding CO and water:
HCOOH = CO + H2O
CO2 + H2 = CO + H2O
(7)
(8)
The observed temperature dependencies are in agreement with early published data on FA decomposition over Pd/ZnO catalyst [8]. At temperatures above 350 °C, negligible amount of methane was produced as a by-product by
hydrogenation of carbon oxides. This observation is in agreement with the course of CO methanation reaction over Pt-containing catalyst [19, 20]:
CO + 3H2 = CH4 + H2O (9)
100 150 200 250 300 350 400 450 Temperature, DC
Fig.1. Effect of temperature on formic acid conversion and product selectivity (H2, CO, CO2, CH4) in FA decomposition over Pt/CeO2-ZrO2 catalyst. Reaction conditions: P = 1 atm; GHSV = 10000 h-1. Inlet composition: HCOOH:N2 = 10:90 vol. %.
In general, the Pt/CeO2-ZrO2 catalyst demonstrates good performance for FA decomposition into hydrogen-rich gas. It provides 100% FA conversion with high (~ 94 %) H2 and CO2 selectivity at 250-300 °C. With consideration of the results obtained, we calculated the hydrogen-rich gas composition (excluding N2) after the FA decomposition at
250-300 °C (vol. %): 47 H2; 47 CO2; 3 H2O and 3 CO. As stated in [21], a gas mixture of this composition can be used directly for feeding high-temperature polymer electrolyte membrane fuel cells (HT PEMFCs) as well as solid oxide fuel cells (SOFCs) without any cleaning processes.
3.2. Catalytic decomposition of methanol
Unlike formic acid, methanol decomposes over the Pt/CeO2-ZrO2 catalyst with the predominant formation of H2 and CO. Fig. 2 shows temperature dependencies of methanol conversion and the selectivity of the main reaction products (H2, CO, CO2, CH4) in methanol decomposition over Pt/CeO2-ZrO2
catalyst. At 200 °C, methanol conversion was ~20% which increased as temperature increased to reach ~100 % at 300 °C. H2 and CO are main reaction products at 200-300 °C; their selectivity was ~100 % suggesting that the methanol decomposition over Pt/CeO2-ZrO2 proceeds according to reaction (10):
CH3OH = 2H2 + CO
(10)
The high reaction selectivity is consistent with the data reported in previously published works [10].
Then, as the temperature rose above 300 °C, the product distribution changed drastically; the H2 and CO selectivity decreased,
whereas the CH4 and CO2 selectivity increased up to 10 and 40 %, respectively. The formation of CH4, CO2 and H2O (not shown in Fig. 2) is most likely related to consecutive proceeding of CO hydrogenation to methane and water (9) and Water Gas Shift (WGS) reaction (11):
CO + H20 = H2 + C02
(11)
Fig. 2. Effect of temperature on methanol conversion and product selectivity (H2, CO, CO2, CH4) in methanol decomposition over Pt/CeO2-ZrO2 catalyst. Reaction conditions: P =1 atm; GHSV = 10000 h-1. Inlet composition: CH3OHN = 10:90 vol. %.
Thus, Fig. 2 data show that Pt/CeO2-ZrO2 is effective for methanol decomposition into hydrogen-rich gas. Moreover, the catalyst demonstrates good stability during the reaction.
The results obtained prove that methanol decomposition over the Pt/CeO2-ZrO2 catalyst is quite promising for efficient production of synthesis gas for SOFC feeding applications.
3.3. Catalytic decomposition of DMM and DME
Fig. 3 illustrates the effect of temperature on the conversion and product selectivity in DMM and DME decomposition reactions over Pt/CeO2-ZrO2 catalyst. As is seen in Fig. 3, the DMM and DME conversions over Pt/CeO2-
ZrO2 catalyst proceed in a higher temperature region as compared to FA and methanol decomposition. Moreover, the temperature dependencies of the conversion and product distribution for DMM decomposition were
similar to those for DME decomposition. In particular, at 300 °C the DMM and DME conversions did not exceed 20%, increased with temperature, and reached ~100 % at temperatures above 400 °C yielding H2, CO, CH4 and CO2 were as the main reaction products for both DMM and DME decomposition reactions. The selectivities of water, ethylene and methanol were negligibly low and are not shown in Fig. 3. At 300 °C, H2 and CO were the main products (S > 60 %) of DMM and DME decomposition reactions. Then,
as the reaction temperature increased, the product distribution changed strongly: H2 and CO selectivity decreased from 60-70% to 2040% with simultaneous increase in CH4 formation up to 50-70 %. Note that the CO2 selectivity increased as temperature rose, but didn't exceed 15% even at 400-450 0 C. Similarly to methanol decomposition (Fig. 2), the regularities of product distribution presented in Fig. 3 can be associated with the formation of CH4 and C02 by, for example, side-reactions (9) and (11).
Fig. 3. Effect of temperature on DMM (a) and DME (b) conversion and product selectivity (H2, CO, CO2, CH4) in DMM (a) DME (b) decomposition over Pt/CeO2-ZrO2 catalyst. Reaction conditions: P = 1 atm; GHSV = 10000 h-1. Inlet composition: CH3OCH2OCH3 :N2 = 10:90 vol. % for DMM decomposition and CH3OCH3:N2 = 10:90 vol. % for DME decomposition.
In general, the data in Fig. 3 indicate that the reactions of DMM and DME decomposition on Pt/CeO2-ZrO2 are less efficient than FA and methanol decomposition, and even than DMM and DME steam reforming [9, 14]. The most likely explanation to this fact is that the temperature of complete DMM and DME conversion coincides with the temperature of side reaction of CO methanation. The hydrogen-rich gas mixture with high content of methane resulting from DMM and DME decomposition reactions can be used for SOFC feeding but the efficiency of SOFC operation with such a fuel stays behind that of SOFC fuelled by pure hydrogen [22].
In addition, during DMM and DME decomposition experiments (Fig. 3), deactivation of the Pt/CeO2-ZrO2 catalyst was observed. The catalyst performance before and after the cycles of reaction temperature increase-decrease was different. Fig. 4 shows the effect of time on-stream on the DMM and
DME conversions (a), the H2 productivity (b) in decomposition of DMM (1) and DME (2) over the Pt/CeO2-ZrO2 catalyst. Obviously, the catalyst provided stable operation during 5 h at 350 °C. As Fig. 4 shows, during the first hour on-stream, the Pt/CeO2-ZrO2 demonstrated continuous deactivation in both DMM and DME decomposition reactions: DMM conversion decreased from 68 to 55 % and DME conversion - from 39 to 31 % (Fig. 4a); H2 productivity - from ~1.3 to 1 L/(gcat • h) and from 0.4 to 0.33 L/(gcat • h) (Fig. 4a), respectively, for DMM and DME decomposition. Then the conversions and H2 productivity remained almost unchanged with time. The TPO studies of the catalysts after DMM and DME decomposition reactions for 5 h revealed carbon formation in the amounts of 0.8 and 0.43 wt. % (to the weight of the catalyst), respectively. Note that the carbon deposition was proportional to the conversion values. In addition, comparative analysis (Fig.
4) shows that Pt/CeO2-ZrO2 decomposes DMM almost twice exceeds that of DME, H2 more efficiently than DME: DMM conversion productivity - 3 times.
Fig.4. Effect of time-on-stream on conversion (a) and H2 productivity (b) in DMM (1) and DME (2) decomposition over Pt/CeO2-ZrO2 catalyst. Reaction conditions: P = 1 atm; T = 350 0C; GHSV = 10000 h-1. Inlet composition: CH3OCH2OCH3N = 10:90 vol. % for DMM decomposition and CH3OCH3:N2 = 10:90 vol. % for DME decomposition.
Although the Pt/CeO2-ZrO2 catalyst was improve its activity and stability, and not sufficiently stable during DMM and DME understand in more details the reaction decomposition to hydrogen-rich gas, it seems mechanism. reasonable to perform further studies in order to
3.4. Comparison of Pt/CeO2-ZrO2 performance in FA, methanol, DMM and DME decomposition reactions
Finally, it seems reasonable to the temperature of complete conversion of
summarize the Pt/CeO2-ZrO2 performance in oxygenates into H2-containing gas;
FA, methanol, DMM and DME decomposition environmental safety of feedstock; main
reactions. Table 1 presents the following data: reaction products; favorable fuel cell type.
Table 1. Performance of the Pt/CeO2-ZrO2 catalyst in FA, methanol, DME and DMM decomposition to hydrogen-rich gas.
Type of fuel Safety T, oC Main products Favorable fuel cells
Formic acid Corrosiveness 200-300 H2, CO2 HT PEMFCs* SOFCs**
Methanol Toxity 250-300 H2, CO SOFCs
Dimethyl ether Nontoxic, noncorrosive 400 CH4, H2, CO SOFCs
Dimethoxymethane Nontoxic, noncorrosive 400 CH4, H2, CO SOFCs
* HT PEMFCs - high temperature polymer electrolyte membrane fuel cells;
** SOFCs - solid oxide fuel cells.
As shown in Table 1, FA and methanol, despite their corrosiveness and toxicity, decompose with high efficiency into hydrogen-rich gas over the Pt/CeO2-ZrO2 catalyst at relatively low temperatures (< 300 0C). Note again that hydrogen-rich gas produced by FA decomposition is suitable for feeding both HT PEMFCs and SOFCs, while that generated by methanol decomposition - only for SOFC feeding.
On the contrary, DMM and DME, being
environmentally friendly compounds, demonstrated low hydrogen productivity in decomposition reactions over the Pt/CeO2-ZrO2 catalyst. Complete conversion of DMM and DME was achieved at higher temperatures (~400 oC). Moreover, regardless the feedstock type (DMM, DME), the catalyst yielded hydrogen-containing gas with high methane content which can also be used directly to feed SOFCs.
Conclusions
Catalytic decomposition of formic acid, methanol, DMM and DME into hydrogen-rich gas was investigated over 1.9 wt.% Pt/CeO2-ZrO2 catalyst at 150-450 0 C, atmospheric pressure, GHSV = 10000 h-1 and feedstock:^ = 10:90 (vol.%).
Comparative investigations show that formic acid and methanol decomposition reactions are more efficient than DMM and DME decomposition. The Pt/CeO2-ZrO2 catalyst provided complete conversion of formic acid and methanol to hydrogen-rich gas with
high H2 selectivity (> 94 %) at 250-300 °C. Unlike formic acid and methanol, DMM and DME decompose over the Pt/CeO2-ZrO2 catalyst at higher temperatures ~400 °C, so produced hydrogen-rich gas contains significant amount of methane. The Pt/CeO2-ZrO2 catalyst was not sufficiently stable in DMM and DME decomposition reactions. Therefore, our further studies are aimed at developing a more active and stable catalyst and probable mechanism of DMM and DME decomposition.
Acknowledgements
This work was supported by the Ministry of Science and Higher Education of the Russian Federation (Project AAAA-A17-117041710088-0).
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КАТАЛИТИЧЕСКОЕ РАЗЛОЖЕНИЕ КИСЛОРОДСОДЕРЖАЩИХ ОРГАНИЧЕСКИХ СОЕДИНЕНИЙ ХИМИИ С1 В ВОДОРОДСОДЕРЖАЩИЙ ГАЗ
С.Д. Бадмаев1'2, А.Е. Пинигина1'2, В.Д. Беляев1, В.А. Собянин1
1 Институт катализа им. Г.К. Борескова Сибирского отделения РАН, пр. Лаврентьева 5, г. Новосибирск, 630090 Россия 2 Новосибирский государственный университет, ул. Пирогова 2, г. Новосибирск, 630090 Россия e-mai\:sukhe@catalysis. ги
Аннотация: Исследованы реакции каталитического разложения кислородсодержащих органических соединений химии С1 в водородсодержащий газ на катализаторе Р1/Се02-2г02. Показано, что этот катализатор при атмосферном давлении и температуре до 450 оС обеспечивает полное разложение муравьиной кислоты, метанола, диметоксиметана и диметилового эфира. Обсуждаются преимущества и недостатки каждой реакции для получения водородсодержащего газа для питания топливных элементов.
Ключевые слова: Каталитическое разложение, оксигенаты, соединения химии С1, муравьиная кислота, метанол, диметоксиметан и диметиловый эфир, платина, водород, синтез газ.
Ci OKSÎGENT3RKÎBLÎ UZVÎ BÎRL3§M3L3RÎN HÎDROGENT3RKÎBLÎ QAZLARA
KATALÎTÎK PARÇALANMASI
S.D. Badmayev1'2, A.E. Pinigina1'2, V.D. Belyayev \ V.A. Sobyanin1
1REA Sibir §ôbssi, G.K. Boreskov adina Kataliz institutu. Lavrentieva prospekti 5, Novosibirsk, 630090 Rusiya 2Novosibirsk Dôvlst Universiteti, Pirogova kuç. 2, Novosibirsk, 630090 Rusiya e-mail:sukhe@catalysis. ru
C1 oksigentarkibli uzvi birlaçmalarin Pt/CeO2-ZrO2 katalizatorun içtiraki ils hidrogentarkibli qazlara katalitik parçalanma reaksiyasi tadqiq olunub. Gostalilib ki, bu katalizator atmosfer tazyiqinda va 450 0C temperaturda qariçqa turçusunun, metanolun, dimetoksimetanin va dimetilefirin tam parçalanmasini tamin edir. Yanacaq elementlari uçun hidrogen qazinin alinmasinda bu reaksiyalarin har birinin ustunluyu va çatiçmayan cahatlari muzakira olunub.
Açar soztar: katalitik parçalanma, qariçqa turçusu, metanol, dimetoksimetan, dimetilefiri, platin, hidrogen.
