CN115341221A - Method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline condition in coupling manner - Google Patents
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- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 title claims abstract description 123
- 235000019445 benzyl alcohol Nutrition 0.000 title claims abstract description 41
- 239000001257 hydrogen Substances 0.000 title claims abstract description 25
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 25
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 23
- 238000000034 method Methods 0.000 title claims abstract description 16
- 238000006056 electrooxidation reaction Methods 0.000 title claims abstract description 9
- 230000008878 coupling Effects 0.000 title claims abstract description 4
- 238000010168 coupling process Methods 0.000 title claims abstract description 4
- 238000005859 coupling reaction Methods 0.000 title claims abstract description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 38
- 238000006243 chemical reaction Methods 0.000 claims abstract description 37
- 239000003054 catalyst Substances 0.000 claims abstract description 21
- 239000011259 mixed solution Substances 0.000 claims description 11
- 239000008151 electrolyte solution Substances 0.000 claims description 6
- FBMUYWXYWIZLNE-UHFFFAOYSA-N nickel phosphide Chemical compound [Ni]=P#[Ni] FBMUYWXYWIZLNE-UHFFFAOYSA-N 0.000 claims description 5
- 239000002105 nanoparticle Substances 0.000 claims description 4
- WVDDGKGOMKODPV-ZQBYOMGUSA-N phenyl(114C)methanol Chemical compound O[14CH2]C1=CC=CC=C1 WVDDGKGOMKODPV-ZQBYOMGUSA-N 0.000 claims description 3
- WPYMKLBDIGXBTP-UHFFFAOYSA-N benzoic acid Chemical compound OC(=O)C1=CC=CC=C1 WPYMKLBDIGXBTP-UHFFFAOYSA-N 0.000 abstract description 18
- 239000006260 foam Substances 0.000 abstract description 11
- 239000005711 Benzoic acid Substances 0.000 abstract description 9
- 235000010233 benzoic acid Nutrition 0.000 abstract description 9
- 229910052759 nickel Inorganic materials 0.000 abstract description 6
- 239000000126 substance Substances 0.000 abstract description 3
- 238000004519 manufacturing process Methods 0.000 description 7
- 230000003647 oxidation Effects 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 7
- 230000003197 catalytic effect Effects 0.000 description 6
- 238000010586 diagram Methods 0.000 description 6
- HUMNYLRZRPPJDN-UHFFFAOYSA-N benzaldehyde Chemical compound O=CC1=CC=CC=C1 HUMNYLRZRPPJDN-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 238000004817 gas chromatography Methods 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 229910021607 Silver chloride Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 238000002848 electrochemical method Methods 0.000 description 2
- 238000000157 electrochemical-induced impedance spectroscopy Methods 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- QNGNSVIICDLXHT-UHFFFAOYSA-N para-ethylbenzaldehyde Natural products CCC1=CC=C(C=O)C=C1 QNGNSVIICDLXHT-UHFFFAOYSA-N 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 239000012670 alkaline solution Substances 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 238000010349 cathodic reaction Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000001627 detrimental effect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000010411 electrocatalyst Substances 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000001075 voltammogram Methods 0.000 description 1
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- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
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Abstract
The invention provides a method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline conditions in a coupling way, which is characterized in that the following reactions respectively occur at an anode and a cathode: and (3) anode reaction: 2RCH 2 OH+6OH － →2RCO 2 H+4H 2 O+6e － And (3) cathode reaction: 6H 2 O+6e － →3H 2 +6OH － . In the invention, ni is used 2 P/NF (NF refers to nickel foam) catalyzes benzyl alcohol to obtain benzoic acid, the conversion efficiency is very high, and the invention uses the same catalyst Ni 2 Hydrogen is produced by the P/NF cathode, benzoic acid is obtained by the anode, and hydrogen energy and chemicals with high added values can be obtained simultaneously.
Description
Technical Field
The invention relates to the technical field of electrocatalysis. More particularly, relates to a method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline conditions.
Background
Hydrogen (H2) has been widely recognized as an environmentally friendly, sustainable energy source to mitigate fossil fuel consumption and associated environmental crisis. Electrocatalytic hydrogen production is one of the most promising strategies, but traditional electrocatalytic water splitting still faces the following major challenges: (I) The Oxygen Evolution Reaction (OER) at the anode is detrimental to the kinetics and thermal processes of the overall reaction, which severely affects the overall reaction efficiency; (II) Simultaneous production of H 2 And O 2 The formation of dangerous explosive mixtures severely hampers the practical application of water electrolysis. Although ion or proton exchange membranes are used to separate the cathode and anode, such modifications increase operating and equipment costs.
Therefore, the development of cheap and efficient electrocatalysts, the assembly of the membraneless electrolytic cell and the simultaneous acquisition of hydrogen energy and high value-added chemicals are of great significance.
Disclosure of Invention
The invention aims to solve the problems and provides a method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline conditions.
In order to achieve the purpose, the technical scheme of the invention is as follows:
the method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline condition is characterized in that the following reactions respectively occur at an anode and a cathode:
and (3) anode reaction: 2RCH 2 OH+6OH － →2RCO 2 H+4H 2 O+6e － ，
And (3) cathode reaction: 6H 2 O+6e － →3H 2 +6OH － 。
Further, the anodic reaction and the cathodic reaction both use nickel phosphide nanoparticles (Ni) 2 P/NF) as a catalyst.
Further, the electrolyte solution is a mixed solution of KOH and benzyl alcohol, the concentration of KOH in the mixed solution is 1M, and the concentration of benzyl alcohol in the mixed solution is 50mM.
By adopting the technical scheme, the invention has the following beneficial effects:
(1) Compared with the traditional industrial process, the electrocatalytic benzyl alcohol oxidation conforms to 'green chemistry', does not have harsh reaction conditions and complicated separation steps, and uses Ni 2 The P/NF catalyzes the benzyl alcohol to obtain the benzoic acid, and the conversion efficiency is very high.
(2) The cathode of the invention produces hydrogen, and the anode obtains benzoic acid, and can simultaneously obtain hydrogen energy and chemicals with high added value.
(3) The invention does not need to use ion or proton exchange membranes to separate the cathode and the anode, thereby reducing the cost.
(4) The invention uses the mixed solution of KOH and benzyl alcohol as the electrolyte solution, can reduce the driving potential, can greatly reduce the industrial electric energy loss, and can obtain the oxidation product with high added value.
Drawings
Fig. 1 and 2 are electrochemical characterization diagrams.
Fig. 3 is an electrochemical impedance diagram.
Fig. 4 and 5 are electrochemical stability diagrams.
FIG. 6 is a graph of the conversion of benzyl alcohol.
FIG. 7 is a graph of the conversion of benzyl alcohol over different catalyst systems.
Fig. 8 and 9 are electrochemical characterization diagrams of two-electrode systems.
Detailed Description
It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not limiting of the invention.
Example (b): the invention uses a mixed solution of KOH and benzyl alcohol as an electrolyte solution, wherein the concentration of KOH in the mixed solution is 1M, and the concentration of the benzyl alcohol in the mixed solution is 50mM.
Using nickel phosphide nanoparticles (Ni) 2 P/NF, where NF refers to nickel foam) as a catalyst, catalyzes the cathodic hydrogen production reaction, and catalyzes the anodic benzyl alcohol to benzoic acid reaction. Especially the reaction for preparing the benzoic acid by the catalytic anode has the efficiency far higher than that of other catalysts.
The invention has the following reactions at the anode and the cathode:
and (3) anode reaction: 2RCH 2 OH+6OH － →2RCO 2 H+4H 2 O+6e － ，
And (3) cathode reaction: 6H 2 O+6e － →3H 2 +6OH － 。
Next, in the electrochemical workstation, a silver/silver chloride electrode was used as a reference electrode, a graphite electrode was used as a counter electrode, and Ni 2 The P/NF was used as the working electrode to form a three-electrode system, and the mixed solution of KOH and benzyl alcohol was used as the electrolyte solution to test the activity of hydrogen production and benzyl alcohol oxidation on the working electrode (see FIGS. 1 to 7).
The electrocatalysis test of the embodiment of the invention is carried out at Chenghua 760E workstation, and the sweep rate for LSV scanning is 5 millivolts per second. The nickel foam used for the synthesis catalyst had dimensions of 1cm by 2cm, while the area of the working electrode was 1cm by 1cm. The oxidation product of the electrocatalysis system is detected by GC-7920 gas chromatography of Beijing Zhongzhijin source science and technology Limited, wherein 5A molecular sieve columns and a thermal conductivity cell detector (TCD) are used for the gas chromatography, and argon is used as a carrier gas. The conversion of benzyl alcohol is calculated by the formula: benzyl alcohol conversion = moles of benzyl alcohol reacted/initial moles of benzyl alcohol. Method for calculating faradaic efficiency of benzyl alcohol (FE): faradaic efficiency = (m × n × F)/(I × t), where F is the faradaic constant (96485C mol-1), n is the number of electron transfers to product, m is the number of moles of product, I is the current, and t is the time.
Wherein the catalyst is nickel phosphide nanoparticles (Ni) 2 P/NF) is synthesized by the following method: putting the cut nickel foam with the size of 1cm multiplied by 2cm into a tubular furnace for phosphorization at the temperature of 300 ℃ for 2 hours.
Overpotential at different current densities can be obtained from a Linear Sweep Voltammogram (LSV), and the obtained voltage is relative to RHE, and the conversion relationship is that E (V vs RHE) = E (Ag/AgCl) +0.197+0.059pH (as shown in FIG. 1 and FIG. 2);
electrochemical impedance spectroscopy measurements were recorded at a corresponding potential of 0.001-10000 Hz with an amplitude of 10mV and a potential of-0.45V vs RHE. The electrochemical impedance is related to the electron transport properties of the catalyst, and the smaller the electrochemical impedance, the faster the electron transport and the more favorable the catalytic reaction. Electrochemical Impedance (EIS) measurements As shown in FIG. 3, ni of the present invention was present in all samples 2 Minimum radius of P/NF circle, charge transfer resistance (R) ct ) The value is 3.381 Ω, indicating Ni compared to the other catalysts 2 The P/NF electrochemical impedance is minimum, and the electron transfer rate is fastest.
The present invention compares catalytic activity between different catalysts, including Ni foam (e.g., ni foam in FIG. 1), niO (e.g., niO in FIG. 1), ni 3 S 2 (Ni in FIG. 1) 3 S 2 ) 20% of C-containing Pt (e.g. Pt/C (20%) in FIG. 1)), irO 2 (IrO as in FIG. 1) 2 ) And Ni of the invention 2 P/NF (as Ni in FIG. 1) 2 P)。
FIGS. 1 and 2 are LSV diagrams of oxidation and hydrogen evolution, and it can be seen that Ni of the present invention 2 P/NF showed excellent catalytic performance relative to other catalysts, as shown in FIG. 1, ni in the absence of benzyl alcohol 2 The P/NF required 1.39V vs. RHE voltage to reach 30mA cm -2 The current density of (2) was 30mA cm driven when 50mM benzyl alcohol was added -2 The potential only needs 1.32V vs. RHE, so that the industrial electric energy loss can be greatly reduced, and meanwhile, the oxidation product with high added value can be obtained. When changing the anion P to S or O, we get Ni 3 S 2 Or NiO, ni 3 S 2 The potentials of the NiO/NF and the NiO/NF are respectively 1.35V vs. RHE and 1.37V vs. RHE, and the noble metal base I rO 2 The catalytic performance of the/NF (1.61V s.RHE) and the nickel foam (1.65V s.RHE) is also obviously lower than that of N i 2 P/NF. As shown in FIG. 2, ni is generated during hydrogen evolution 2 The P/NF catalyst only needs 99mV vs. RHE voltage to drive 10mA cm -2 Current density of (2), ni 2 P/NF in 50mM benzylThe LSV curves for alcohol and no benzyl alcohol did not change much, indicating that benzyl alcohol has a very weak effect on HER in alkaline solution. In addition, with Pt/C (20mV vs. RHE), ni 3 S 2 Comparative studies were also performed on/NF (157mV vs. RHE), niO/NF (219mV vs. RHE) and Nifoam (377mV vs. RHE), ni 2 P/NF showed excellent hydrogen evolution activity. The stability of the catalyst of the present invention in 7 cycles of the reaction system and the stability in the hydrogen evolution reaction are shown in fig. 4 and 5, fig. 4 shows that the conversion rate of the benzyl alcohol is not lower than 96% (96% -99%), the faradaic efficiency is not lower than 93%, and the catalyst Ni used in the present invention is proved 2 The P/NF has high catalytic performance and high stability, and in the long-time hydrogen evolution process (figure 5), the catalyst can be maintained for 500 hours (about 21 days), and the performance is not degraded, which shows that the nickel phosphide has good electrochemical stability in the strong alkaline harsh electrolyte, and has very large application prospect in industry.
Through gas chromatography, a conversion diagram of the benzyl alcohol, the benzoic acid and the benzaldehyde is obtained, as shown in fig. 6, in the catalysis process, the raw material benzyl alcohol is gradually reduced, the benzoic acid is increased, the content of the benzaldehyde is always relatively low, and finally the benzyl alcohol is almost completely converted into the benzoic acid. FIG. 7 comparison of different catalysts, ni 2 The conversion rate of P/NF benzyl alcohol is up to 99.3%, besides, we also studied Ni foam, niO/NF and Ni 3 S 2 Benzyl alcohol conversion of/NF, as shown in FIG. 7, ni 2 The conversion rate of P/NF benzyl alcohol is far higher than that of Ni foam (7.99%), niO/NF (33.01%) and Ni 3 S 2 /NF(77.17％)。
In a three-electrode system, the Ni2P/NF catalyst provided by the invention has good catalytic reduction hydrogen production and benzyl alcohol oxidation activities. Based on the method, the invention constructs the method based on Ni 2 The activity of hydrogen production and benzyl alcohol oxidation was tested simultaneously in a two-electrode cell with P/NF as both anode and cathode catalysts, using the mixed KOH and benzyl alcohol solution as the electrolyte solution, as shown in fig. 8.
As shown in FIG. 8, we also refer to Ni 3 S 2 Comparison was made of/NF, niO/NF and Nickel foam (Nifoam), ni 3 S 2 The potentials required for the/NF, niO/NF and Ni foams were 1.51V,1.73V and 1.86V to reach 10mA cm -2 Current density of (2) is obviously lower than that of Ni 2 P/NF，Ni 2 The P/NF only needs 1.45V to generate 10mA cm -2 The catalytic current density of (2) is much lower than the voltage (1.61V) in the fully decomposed water. In addition, to Ni 2 The P/NF catalyst was subjected to 5 cycles to evaluate its stability. As shown in FIG. 9, the conversion of benzyl alcohol was not less than 97%, indicating that Ni was not present 2 The P/NF catalyst has stronger stability.
It will be evident to those skilled in the art that the invention is not limited to the details of the foregoing illustrative embodiments, and that the present invention may be embodied in other specific forms without departing from the spirit or essential attributes thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein.
Furthermore, it should be understood that although the present description refers to embodiments, not every embodiment may contain only a single embodiment, and such description is for clarity only, and those skilled in the art should integrate the description, and the embodiments may be combined as appropriate to form other embodiments understood by those skilled in the art.
Claims (3)
1. The method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline condition is characterized in that the following reactions respectively occur at an anode and a cathode:
and (3) anode reaction: 2RCH 2 OH+6OH － →2RCO 2 H+4H 2 O+6e － ，
And (3) cathode reaction: 6H 2 O+6e － →3H 2 +6OH － 。
2. According to the rightThe method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline condition coupled with claim 1, wherein nickel phosphide nanoparticles (Ni) are used for the anode reaction and the cathode reaction 2 P/NF) as a catalyst.
3. The method for preparing hydrogen by electrooxidation of benzyl alcohol under alkaline conditions through coupling of claim 1, wherein the electrolyte solution is a mixed solution of KOH and benzyl alcohol, the concentration of KOH in the mixed solution is 1M, and the concentration of benzyl alcohol in the mixed solution is 50mM.
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| CN114438542A (en) * | 2022-01-24 | 2022-05-06 | 北京工业大学 | Preparation method of nickel nanowire array electrode loaded nickel manganese phosphide active layer and application of nickel nanowire array electrode loaded nickel manganese phosphide active layer in electrocatalysis of benzyl alcohol |
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| Title |
|---|
| BO YOU ET AL.: "Efficient H2 Evolution Coupled with Oxidative Refining of Alcohols via A Hierarchically Porous Nickel Bifunctional Electrocatalyst", 《ACS CATALYSIS》, 30 May 2017 (2017-05-30), pages 4564 - 4570 * |
| BO YOU ET AL.: "Electrocatalytic and photocatalytic hydrogen evolution integrated with organic oxidation", 《CHEMCOMM》, 3 May 2018 (2018-05-03), pages 5943 * |
| BO YOU ET AL.: "Simultaneous H2 Generation and Biomass Upgrading in Water by an Efficient Noble-Metal-Free Bifunctional Electrocatalyst", 《ANGEW. CHEM. INT. ED.》, 15 July 2016 (2016-07-15), pages 9913 - 9917 * |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114438542A (en) * | 2022-01-24 | 2022-05-06 | 北京工业大学 | Preparation method of nickel nanowire array electrode loaded nickel manganese phosphide active layer and application of nickel nanowire array electrode loaded nickel manganese phosphide active layer in electrocatalysis of benzyl alcohol |
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