CN105406032A - Preparation method of hydrogen storage alloy and nano-porous nickel composite (HSAs/NPNi) and application thereof - Google Patents
Preparation method of hydrogen storage alloy and nano-porous nickel composite (HSAs/NPNi) and application thereof Download PDFInfo
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- CN105406032A CN105406032A CN201510996773.4A CN201510996773A CN105406032A CN 105406032 A CN105406032 A CN 105406032A CN 201510996773 A CN201510996773 A CN 201510996773A CN 105406032 A CN105406032 A CN 105406032A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/24—Electrodes for alkaline accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/24—Electrodes for alkaline accumulators
- H01M4/242—Hydrogen storage electrodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/24—Electrodes for alkaline accumulators
- H01M4/26—Processes of manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to a preparation method of an AB5 type hydrogen storage alloy (HSAs) and a nano-porous nickel (NPNi) composite (HSAs/NPNi) and an application thereof as a negative material of a nickel-metal hydride battery. The HSAs/NPNi composite is prepared through a simple hydrothermal method and a subsequent annealing treatment. The specific preparation steps are as follows: step a, under the protection of argon, smelting a rare earth element and other metallic elements by an electric arc furnace, and obtaining an ingot; step b, under the protection of argon, annealing and mechanically polishing the ingot, and obtaining an alloy powder, wherein the average particle diameter of the alloy powder is 50 mum; step c, using the simple hydrothermal method to prepare an Ni(OH)2 powder; and step d, integrating the prepared Hi(OH)2 and HSAs, drying the mixture in an electric dry oven, then in an Ar/H2 mixed gas atmosphere, annealing in a tube furnace and restoring the Ni(OH)2, and then the HSAs/NPNi composite can be prepared. As the negative material of the nickel-metal hydride battery, the composite has excellent high-rate discharge performance; and when the discharge current density is 3,000 mAg-1, the capacity retention rate of the composite can reach up to 43.11%, which is 3.2 times of a separate hydrogen storage alloy electrode.
Description
Technical field:
The present invention relates to the preparation of HSAs/NPNi composite material and the application as nickel-hydrogen battery negative pole material thereof.
Background technology:
In recent years, along with environmental problem is increasingly serious, the continuous aggravation of energy crisis, new-energy automobile receives increasing concern.Electric automobile (EV), mixed power electric car (HEV) and fuel cell electric vehicle (FCVs) are the main bodys of new-energy automobile.And the key developing EVs, HEVs and FCVs is exactly the application of high efficiency, low cost, safety, environmentally friendly battery.As everyone knows, good battery performance is the key realizing being changed by oil gas epoch to the electric power epoch.The battery technology of some advanced persons, such as nickel metal hydride (Ni/MH) battery, lithium ion battery and proton exchange membrane (PEM) fuel cell etc., be widely used in mobile electronic device, electric tool, electric automobile etc.And Ni-MH battery due to its low cost, long-life and excellent fail safe and thermal adaptability be the first-selection of Hybrid Vehicle battery.The requirement of above-mentioned application to Ni-MH battery energy density is relatively low, then very high to the requirement of power density.In addition, electric tool is also very high to the requirement of power density with some modern military equipment.Therefore, in order to meet the demand of market to high-capacity nickel-hydrogen battery, improving the competitiveness of Ni-MH battery further, constantly must improve the high-rate discharge ability (HRD) of hydrogen bearing alloy.
Summary of the invention:
The object of this invention is to provide a kind of preparation of HSAs/NPNi composite material and the application as nickel-hydrogen battery negative pole material thereof.Relate to a kind of AB
5type hydrogen storage alloy (HSAs) and the preparation method of nanoporous nickel (NPNi) composite material (HSAs/NPNi) and the application as nickel-hydrogen battery negative pole material thereof.This invention has prepared HSAs/NPNi composite material by simple hydro thermal method and annealing in process subsequently.The architectural characteristic of this composite material uniqueness makes it have electronics and ion transfer speed faster, thus substantially increases its high-rate discharge ability.
Above-mentioned purpose of the present invention is achieved through the following technical solutions, and particular content is as follows:
The preparation method of a kind of hydrogen bearing alloy and nanoporous nickel composite material (HSAs/NPNi), comprises the following steps:
A, in high-purity argon gas atmosphere by lanthanum, cerium, yttrium, nickel, cobalt, manganese, the aluminium of method melting purity >=99.5 of electric arc melting, obtain its ingot casting;
B, to be annealed under argon atmosphere by ingot casting and mechanical lapping obtains master alloy powder, its average particulate diameter is 50 μm;
C, prepare Ni (OH) by simple hydro thermal method
2powder, by 1.4 ~ 1.5gNi (NO
3)
2, the mixture of 1.3 ~ 1.5g hexamethylene tetramine (HMT) and 30 ~ 40ml ultra-pure water joins to be had in teflon-lined stainless steel autoclave; The reactor of sealing is put into 100 ~ 120 DEG C of electric dry oven insulation 10 ~ 12h, by green product Ni (OH)
2pass through collected by centrifugation;
D, by prepared Ni (OH)
2with foundry alloy grind in agate mortar evenly carry out integrated; Mixture is dry in electric dry oven, then at tube furnace Ar/H
2thermal reduction 5 ~ 6h under 400 ~ 450 DEG C of conditions in gaseous mixture atmosphere, preparation HSAs/NPNi composite material.
In described step a, the composition of ingot casting is not only confined to AB
5, also can be AB
2, AB
3type hydrogen storage alloy.
Ni (OH) is prepared in described step c
2time, Ni (NO
3)
2with the different quality that HMT can be same ratio.
In steps d, the Elevated Temperature Conditions of tube furnace is 1 ~ 3 DEG C/min.
Described hydrogen bearing alloy and nanoporous nickel composite material (HSAs/NPNi), it carries out electro-chemical test as electrode material, comprises the following steps:
A, first by 0.25 ~ 0.255g active material, namely HSAs/NPNi composite material or foundry alloy mix with 1.0 ~ 1.02g carbonyl nickel powder, make at the pressure of 8 ~ 20MPa the electrode slice that diameter is 10 ~ 15mm again by tablet press machine, electrode is immersed in 2 ~ 4h in the KOH solution of 25 ~ 35wt%, makes it soak completely before electro-chemical test;
B, electro-chemical test carry out in the three-electrode system of a standard, and the electrode wherein prepared in step a, as work electrode, sinters Ni (OH)
2/ NiOOH electrode is as to electrode, and mercury/mercury oxide (Hg/HgO) electrode is as reference electrode, and the KOH solution of 25 ~ 35wt% is as electrolyte;
C, with described HSAs/NPNi combination electrode as work electrode carry out discharge capacity test carry out on ARBIN battery test system, under room temperature 25 DEG C of conditions, electrode is with 60mAg
-1(0.2C) current density charging 7.5h, leaves standstill 30min, then with 60mAg
-1(0.2C) current density is discharged to cut-ff voltage and reaches-0.74V relative to Hg/HgO reference electrode, circulates and activates for 4 times, reach maximum discharge capacity C
max;
After d, completely activation, carry out high-rate discharge ability test, electrode is with 300mAg
-1(1C) current density charging, then with 300,600,900,1200,1500,2400,3000mAg
-1(10C) current density is discharged to cut-ff voltage respectively :-0.65 ,-0.6, and-0.5 ,-0.45 ,-0.4 ,-0.35 ,-0.3V, this cut-ff voltage is relative to Hg/HgO reference electrode;
E, electrochemical property test carry out on IVIUM electrochemical workstation.Carry out ac impedance measurement when the amplitude relative to OCP is 5mV, the frequency range of test is by 100kHz to 5mHz; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is-5 to 5mV, carries out sweeping speed for the linear polarisation curves of 0.05mV/s and test; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is 0 to 1.5V, carries out sweeping speed for the anodic polarization curves of 5mV/s and test; Under 100% charged state, under the electromotive force step of+500mV relative to Hg/HgO, carry out the test of the current versus time curve of 4000s;
The hydrogen bearing alloy of f, preparation and nanoporous nickel composite material (HSAs/NPNi), as the negative pole of Ni-MH battery, have excellent high-rate discharge ability.Be 3000mAg at discharge current density
-1time, its capacity retention rate, up to 43.11%, is 3.2 times of independent foundry alloy electrode.
Technique effect of the present invention is:
The hydrogen bearing alloy that the present invention obtains and nanoporous nickel composite material (HSAs/NPNi), due to the loose structure of the three-dimensional co-continuous of nanoporous nickel uniqueness in composite material, accelerate the transmission speed of electronics and ion, accelerate the electrochemical reaction rates of electrode surface and the hydrogen atom diffusion velocity of alloy inside, significantly improve its high-rate discharge ability.
Accompanying drawing illustrates:
High-rate discharge ability curve under Fig. 1, different discharge current density.
The optical photograph preparing schematic diagram and electrode slice of Fig. 2, HSAs/NPNi composite material, wherein:
Preparation method's schematic diagram of a, HSAs/NPNi composite material;
The optical photograph of b, use for electrochemical tests electrode slice.
The SEM photo of Fig. 3, foundry alloy.
The SEM photo of Fig. 4, HSAs/NPNi composite material.
The SEM photo of Fig. 5, NPNi.
The TEM photo of Fig. 6, NPNi.
The HRTEM photo of Fig. 7, NPNi.
The XRD diffracting spectrum of Fig. 8, foundry alloy and HSAs/NPNi composite material.
Fig. 9, linear polarisation curves under 50% depth of discharge.
Figure 10, electrochemical impedance collection of illustrative plates under 50% depth of discharge.
Figure 11, anodic polarization curves under 50% depth of discharge.
Figure 12, the anodic current density discharging current-time graph under 100% charged state.
Embodiment
Below in conjunction with example, the specific embodiment of the present invention is described:
Embodiment
Preparation process in the present embodiment and step as follows:
(1) in high-purity argon gas atmosphere, pass through lanthanum, cerium, yttrium, nickel, cobalt, manganese, the aluminium of method melting purity>=99.5 of electric arc melting, obtain its ingot casting; Also mechanical lapping of being annealed under argon atmosphere by ingot casting obtains the powder of foundry alloy, and its average particulate diameter is 50 μm; Ni (OH) is prepared with simple hydrothermal method
2powder, by 1.45gNi (NO
3)
2, the mixture of 1.4g hexamethylene tetramine (HMT) and 35ml ultra-pure water joins to be had in teflon-lined stainless steel autoclave.The reactor of sealing is put into 100 DEG C of electric dry ovens and be incubated 10h, by green product Ni (OH)
2pass through collected by centrifugation;
(2) by prepared Ni (OH)
2with foundry alloy grind in agate mortar evenly carry out integrated.Mixture is dry in electric dry oven, then at tube furnace Ar/H
2thermal reduction 5h under 400 DEG C of conditions in gaseous mixture atmosphere, wherein Elevated Temperature Conditions is 1 DEG C/min, preparation HSAs/NPNi composite material;
(3) by 0.25g active material, namely HSAs/NPNi composite material or foundry alloy mix with 1.0g carbonyl nickel powder, make at the pressure of 8MPa the electrode slice that diameter is 15mm again by tablet press machine, electrode is immersed in 3h in the KOH solution of 30wt%, makes it soak completely before electro-chemical test; Using this electrode slice as work electrode, Ni (OH)
2/ NiOOH sheet is as to electrode, and mercury/mercuric oxide electrode is as reference electrode, and the KOH solution of 30wt% is electrolyte, and the three-electrode system of composition standard carries out electro-chemical test;
(4) HSAs/NPNi combination electrode as work electrode carry out discharge capacity test carry out on ARBIN battery test system.Under room temperature 25 DEG C of conditions, electrode is with 60mAg
-1(0.2C) current density charging 7.5h, leaves standstill 30min, then with 60mAg
-1(0.2C) current density is discharged to cut-ff voltage and reaches-0.74V relative to Hg/HgO reference electrode, circulates and activates for 4 times, reach maximum discharge capacity C
max; Completely after activation, carry out high-rate discharge ability test, electrode is with 300mAg
-1(1C) current density charging, then with 300,600,900,1200,1500,2400,3000mAg
-1(10C) current density is discharged to cut-ff voltage respectively :-0.65 ,-0.6, and-0.5 ,-0.45 ,-0.4 ,-0.35 ,-0.3V, this cut-ff voltage is relative to Hg/HgO reference electrode;
(5) electrochemical property test carries out on IVIUM electrochemical workstation.Carry out ac impedance measurement when the amplitude relative to OCP is 5mV, the frequency range of test is by 100kHz to 5mHz; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is-5 to 5mV, carries out sweeping speed for the linear polarisation curves of 0.05mV/s and test; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is 0 to 1.5V, carries out sweeping speed for the anodic polarization curves of 5mV/s and test; Under 100% charged state, under the electromotive force step of+500mV relative to Hg/HgO, carry out the test of the current versus time curve of 4000s.
The pattern of HSAs/NPNi composite material and structural characterization:
The surface topography of foundry alloy, HSAs/NPNi composite material and NPNi is observed, see Fig. 3-Fig. 5 by ESEM (SEM).Foundry alloy smooth surface is smooth as can be seen from Figure 3.Compared with the smooth surface of foundry alloy, the surface ratio of HSAs/NPNi composite material is more coarse, and alloy surface is by nanoporous nickel coated (see Fig. 4).At H
2in/Ar gaseous mixture atmosphere under 400 DEG C of conditions, Ni (OH)
2be reduced to NPNi, form the hole of three-dimensional co-continuous, its intermediate pore size is about 200nm, and ligament size is about 150nm (see Fig. 5).Fig. 6 is transmission electron microscope (TEM) photo of NPNi, composition graphs 5, Fig. 6 can find out that NPNi has the nano-porous structure of three-dimensional co-continuous, and NPNi ligament presents bi-curved characters and appearances, wherein positive camber forms ligament and negative cruvature and forms nano-pore.Fig. 7 is the HRTEM photo of NPNi, can find out (111), and the interplanar distance that (010) and (200) crystal face is corresponding is respectively 0.203,0.233 and 0.176nm, and with the feature interplanar distance one_to_one corresponding of nickel.Fig. 8 is the XRD collection of illustrative plates of foundry alloy and HSAs/NPNi composite material, and the characteristic diffraction peak of foundry alloy correspond to CaCu
5the hexagonal structure of type.But HSAs/NPNi composite material not only has the hexagonal structure of CaCu5 type, and there is the characteristic peak of nickel.
At ambient temperature, the Electrochemical Characterization of foundry alloy and HSAs/NPNi composite material:
When carrying out electro-chemical test, composite material and these two electrodes of foundry alloy all than being easier to activation, circulating and can reach maximum discharge capacity in 4 weeks.As shown in Figure 1, at all discharge current density I
cunder, the high-rate discharge ability of HSAs/NPNi combination electrode is better than the high-rate discharge ability of foundry alloy, and both gaps are at I
cmore obvious time larger.Be 3000mAg at discharge current density
-1time, the capacity retention rate of composite material is 3.2 times of foundry alloy capacity retention rate.Fig. 9 is the linear polarisation curves of two electrodes under 50% depth of discharge.Surface exchange current density value I
0can be calculated by the slope of figure cathetus.The I of composite electrode
0value is comparatively large, namely to be bordering on its electrochemical reaction rates under poised state faster than foundry alloy electrode.This is because nanoporous nickel plays catalytic action to Hydrogen evolving reaction (HER), the electrochemical reaction rates of electrode surface is accelerated, the loose structure of the three-dimensional co-continuous of nickel porous makes electronics and ion transfer speed accelerate, and then improve the electrochemical kinetics of electrode, improve high-rate discharge ability.Figure 10 is the test result of electrochemical impedance collection of illustrative plates, can see that each collection of illustrative plates is all made up of two semicircles of high frequency region and the straight line of low frequency range.What little and large semicircle reflected respectively is between alloying pellet or contact resistance (R between alloying pellet and current collector (being NPNi here)
c) and the charge transfer resistance (R of electrode
ct).The straight line portion of low frequency range is then main owing to Warburg impedance.Half circular diameter is less, and its impedance is less.Therefore, nanoporous nickel composite material has less R
cand R
cTvalue, the tight interaction in this bicontinuous structure with nanoporous nickel and composite material between nanoporous nickel and hydrogen storage alloy particle is relevant.Figure 11 gives the anodic polarization curves of foundry alloy and HSAs/NPNi composite material.In process of anodic polarization, first current density increases along with the increase of overpotential, then reaches maximum, and this value is defined as limiting current density (I
l).I
lrelevant in the diffusion rate of alloy inside with hydrogen atom, I
lbe worth larger, the diffusion velocity of hydrogen atom is also larger.Large than foundry alloy electrode of the diffusion rate of the hydrogen atom of HSAs/NPNi combination electrode as seen from the figure.Figure 12 is electromotive force step figure, and can find out, initial period, current density sharply declines, and along with the prolongation of time, current density linearly declines.Can be calculated by the linear segment in fitted figure: large than foundry alloy electrode of the hydrogen atom diffusion coefficient of HSAs/NPNi combination electrode.To sum up, HSAs/NPNi composite electrode has surface electrochemistry reaction speed and alloy internal hydrogen atomic diffusion rates faster, effectively improves its high-rate discharge ability.This composite material can be used as the negative material of Ni-MH battery, has good application prospect in high-power battery field.The preparation method that the present invention relates to can also be extended to other hydrogen bearing alloy systems, provides new method and thinking for improving Ni-MH battery high-rate discharge ability further.
Claims (5)
1. a preparation method for hydrogen bearing alloy and nanoporous nickel composite material (HSAs/NPNi), comprises the following steps:
A, in high-purity argon gas atmosphere by lanthanum, cerium, yttrium, nickel, cobalt, manganese, the aluminium of method melting purity >=99.5 of electric arc melting, obtain its ingot casting;
B, to be annealed under argon atmosphere by ingot casting and mechanical lapping obtains master alloy powder, its average particulate diameter is 50 μm;
C, prepare Ni (OH) by simple hydro thermal method
2powder, by 1.4 ~ 1.5gNi (NO
3)
2, the mixture of 1.3 ~ 1.5g hexamethylene tetramine (HMT) and 30 ~ 40ml ultra-pure water joins to be had in teflon-lined stainless steel autoclave; The reactor of sealing is put into 100 ~ 120 DEG C of electric dry oven insulation 10 ~ 12h, by green product Ni (OH)
2pass through collected by centrifugation;
D, by prepared Ni (OH)
2with foundry alloy grind in agate mortar evenly carry out integrated; Mixture is dry in electric dry oven, then at tube furnace Ar/H
2thermal reduction 5 ~ 6h under 400 ~ 450 DEG C of conditions in gaseous mixture atmosphere, preparation HSAs/NPNi composite material.
2. the preparation method of a kind of hydrogen bearing alloy according to claim 1 and nanoporous nickel composite material (HSAs/NPNi), is characterized in that, in described step a, the composition of ingot casting is not limited to AB
5, or AB
2, AB
3type hydrogen storage alloy.
3. the preparation method of a kind of hydrogen bearing alloy according to claim 1 and nanoporous nickel composite material (HSAs/NPNi), is characterized in that, prepares Ni (OH) in described step c
2time, Ni (NO
3)
2with the different quality that HMT is same ratio.
4. the preparation method of a kind of hydrogen bearing alloy according to claim 1 and nanoporous nickel composite material (HSAs/NPNi), is characterized in that, in steps d, the Elevated Temperature Conditions of tube furnace is 1 ~ 3 DEG C/min.
5. the hydrogen bearing alloy that obtains of preparation method according to claim 1 and nanoporous nickel composite material (HSAs/NPNi), it carries out electro-chemical test as electrode material, comprises the following steps:
A, first by 0.25 ~ 0.255g active material, namely HSAs/NPNi composite material or foundry alloy mix with 1.0 ~ 1.02g carbonyl nickel powder, make at the pressure of 8 ~ 20MPa the electrode slice that diameter is 10 ~ 15mm again by tablet press machine, electrode is immersed in 2 ~ 4h in the KOH solution of 25 ~ 35wt%, makes it soak completely before electro-chemical test;
B, electro-chemical test carry out in the three-electrode system of a standard, and the electrode wherein prepared in step a, as work electrode, sinters Ni (OH)
2/ NiOOH electrode is as to electrode, and mercury/mercury oxide (Hg/HgO) electrode is as reference electrode, and the KOH solution of 25 ~ 35wt% is as electrolyte;
C, with described HSAs/NPNi combination electrode as work electrode carry out discharge capacity test carry out on ARBIN battery test system, under room temperature 25 DEG C of conditions, electrode is with 60mAg
-1(0.2C) current density charging 7.5h, leaves standstill 30min, then with 60mAg
-1(0.2C) current density is discharged to cut-ff voltage and reaches-0.74V relative to Hg/HgO reference electrode, circulates and activates for 4 times, reach maximum discharge capacity C
max;
After d, completely activation, carry out high-rate discharge ability test, electrode is with 300mAg
-1(1C) current density charging, then with 300,600,900,1200,1500,2400,3000mAg
-1(10C) current density is discharged to cut-ff voltage respectively :-0.65 ,-0.6, and-0.5 ,-0.45 ,-0.4 ,-0.35 ,-0.3V, this cut-ff voltage is relative to Hg/HgO reference electrode;
E, electrochemical property test carry out on IVIUM electrochemical workstation, and carry out ac impedance measurement when the amplitude relative to Open Circuit Potential (OCP) is 5mV, the frequency range of test is by 100kHz to 5mHz; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is-5 to 5mV, carries out sweeping speed for the linear polarisation curves of 0.05mV/s and test; Under 50% depth of discharge condition, when the potential scan scope relative to OCP is 0 to 1.5V, carries out sweeping speed for the anodic polarization curves of 5mV/s and test; Under 100% charged state, under the electromotive force step of+500mV relative to Hg/HgO, carry out the test of the current versus time curve of 4000s;
The hydrogen bearing alloy of f, preparation and nanoporous nickel composite material (HSAs/NPNi), as the negative pole of Ni-MH battery, have excellent high-rate discharge ability, are 3000mAg at discharge current density
-1time, its capacity retention rate, up to 43.11%, is 3.2 times of independent foundry alloy electrode.
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| CN110013864A (en) * | 2019-04-30 | 2019-07-16 | 西北师范大学 | The preparation of cobalt acid nickel/bismuthyl chloride nano composite material and its application in catalysis reduction organic matter |
| CN110013864B (en) * | 2019-04-30 | 2021-07-27 | 西北师范大学 | Preparation of nickel cobaltate/bismuth oxychloride nanocomposite and application of nanocomposite in catalytic reduction of organic matters |
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