钴镍基材料在碱性溶液中的储能性能研究
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摘要
近年来,一些Co-X(如Co-B、Co-Si、Co-P、Co-S、Co-BN等)材料被发现在碱性体系中具有较高的放电容量和较好的循环稳定性。非活性部分溶解在电解液碱性KOH溶液中,在原有的钴颗粒间形成了大量的空隙,这有利于增大材料与电解液的接触面积,提高了电化学反应的效率,进而对纯Co电极的电化学性能改善起到了非常重要的作用。非金属元素Se具有与上述B、Si、P、S等相似的性质,可以溶解在碱性电解液中,且它的导电性较好,是一种传统的半导体材料,可以推测它在电化学方面具有和上述元素相似的功用,但是目前关于Se在镍基碱性二次电池中的应用却未见报道。
本文采用化学还原法制备了Co-Se复合物,并将其用作碱性二次电池负极材料。放电电流密度为50mAg-1时其放电容量高达380mAhg-1,且循环稳定性良好：130周后,放电容量依然达到356.5mAhg-1,放电容量保持率在93.62%。同等条件下Co电极的放电容量只有130mAhg-1。这主要是由于复合物中的Se提高了Co的分散性能,同时Se在电化学反应过程中逐渐溶解,使电极内产生空隙,增加了Co与电解液接触的面积,提高了电化学反应的效率,进而提高了Co的利用率。对Se在此过程中的作用和反应机理进行了深入探究。
采用物理球磨的方法制备Co-Se-C复合材料并将其用作镍基碱性二次电池负极材料。加入的Se和CNTs较大程度的提高了Co的放电容量,最大放电比容量达到450mAhg-1,同时材料的活化周期明显缩短。这主要是由于Se和CNTs的协同作用,Se的溶解增加了电极活性物质与电解液的接触；而CNTs的引入增加了材料的导电性和韧性。
Co304是一种P型半导体,且其中Co的价态较高,是一种潜在的多电子反应电极材料,我们预测它和CoO、Co(OH)2等一样,有望在镍基碱性二次电池中应用。
本文中采用溶解热和高温煅烧两步法制备了不同形貌的C0304,并将其用作碱性二次电池负极材料。在100mAg-1的电流密度下,多面体C0304最高放电容量能够达到399.9mAh g-1。继续采用降低前驱体煅烧温度的方法,使得材料的比表面积增大,最大放电容量提高至490.2mAhg-1,且循环稳定性良好。对CO3O4电极在充放电过程中的电化学反应机理进行了研究,发现C0304在充电过程中先转化成Co(OH)2,然后继续转化成Co。放电容量主要来源于Co(OH)2与Co的转化。
镍钴氧化物／氢氧化物等由于具有较高的理论放电比容量、价格低廉、电化学氧化还原可逆性好等优点成为较有前途的新型超级电容器材料,目前虽然相关报道较多,但是关于材料的特殊形貌制备和性能研究尚不成体系。本文将以Co3O4、α-Ni(OH)2材料作为研究对象,研究其作为超级电容器电极材料的电化学性能。
采用碳球模板法一步低温水热合成空心C0304微米球。系统研究了在140℃较低温度下前躯体的碳化过程。同时也考察了反应物浓度、反应时间等因素对碳球尺寸、厚度等的影响。采用500℃空气煅烧得到纯度较高的空心Co3O4微米球。研究了C0304的比表面积、孔径等对电化学性能的影响。由于材料具有较大的比表面积和较合适的孔径,在被用作电容器材料时显示了较高的比电容和优异的循环性能。
利用不同的醇和水作混合溶剂,采用溶剂热法制备了不同形貌和比表面积的α-Ni(OH)2。研究了醇的物理性质对材料形貌的影响。当用二缩三乙--醇和水做混合溶剂时,制备的纳米线堆积的α-Ni(OH)2微米球比表面积达到318.6m2g1。在未复合其他材料的情况下,其放电比容量达到1788.9F g-1(放电电流密度为0.5A g-1),且循环性能良好。这主要是由于组成材料的纳米线尺寸较小,这种结构有效缩短了质子扩散路径,离子扩散阻力也很大程度得到了降低。同时材料的比表面积很大,使得电解液能够渗入活性物质内部,活性物质有效接触面积增大,从而提高了电化学反应效率。
A series of Co-X materials, such as Co-B, Co-Si, Co-P, Co-S, Co-BN and so on, are reported to demonstrate high discharge capacity and excellent cycle stability in alkaline rechargeable batteries. The inactive part can dissolve in alkaline aqueous, resulting in the creation of newly built interspaces among the Co particles. These newly built interspaces can increase the contact area between the active electrode materials of the electrodes and alkaline electrolyte. Thus the efficiency of electrochemical reactions is enhanced, resulting in better electrochemical performance than pure Co. As we know, Selenium can also dissolve in alkaline solutions, which is similar with B, Si, P and S. Besides, the electric conductivity of selenium is better than the above-mentioned elements. It is expected that Se has similar functions in electrochemical application. However, report on its application in alkaline rechargeable batteries has not been found.
Co-Se composite is prepared through a chemical-reduction method and used as the negative electrode material of alkaline rechargeable batteries. The Co-Se composite shows a maximum discharge capacity of380mAh g-1at a current density of50mA g-1. After130cycles, the discharge capacity can still remain at356.5mAh g-1, with a retention rate of93.62%. As a comparison, the discharge capacity of pure Co is only130mAh g-1. This phenomenon can be explained as follows:the incorporation of Se improves the dispersibility of Co in the electrode. In addition, Se dissolves in the alkaline electrolytes, leading to more interspaces in the electrode, which is beneficial for increasing the contact area between the active materials and the electrolytes, thus enhances the efficiency of electrochemical reactions. Effect and function mechanism of Se in the electrochemical process are investigated in-depth.
Co-Se-C composite is prepared through ball-milling method and used as the negative electrode material of alkaline rechargeable batteries. The discharge capacity of Co is obviously improved after the incorporation of Se and CNTs. The maximum discharge capacity of it can reach450mAh g-1at the discharge current density of50 mA g-1. Besides, the cycle number needed to reach the maximum discharge capacity is decreased. This can be attributed to the synergetic effect of Se and CNTs. The dissolution of Se enhances the effective contact between the active material and the electrolytes; whereas the introduction of CNTs improves the conductivity and toughness of the material.
Co3O4is an important P-type semiconductor, in which the average valence of Co is8/3. So it is a potential multi-electron electrode material in alkaline rechargeable batteries. It is expected to display excellent performance as Co(OH)2and CoO.
Co3O4with different morphologies are prepared by a solvothermal/calcination method. Their electrochemical performances as electrode materials of alkaline rechargeable batteries are investigated. The maximum discharge capacity of Co3O4polyhedrons can reach399.9mAh g-1at the discharge current density of100mA g-1. By lowering the calcination temperature, the BET surface area of the sample is enlarged and the electrochemical discharge capacity is increased. The maximum discharge capacity reaches490.2mAh g-1. And the cycle performance is excellent. Reaction mechanism of Co3O4during electrochemical performance is discussed in detail. Co3O4first changes to Co(OH)2in the charged state and then to Co. Faradaic reaction between Co and Co(OH)2accounts for most of the discharge capacity.
Owing to their relative high specific capacitance, excellent reversible redox behavior and low cost, Cobalt/Nickel oxides and hydroxides have been considered as new types of supercapacitor electrode materials. Although many reports have been focused on them, preparation of materials with particular morphologies and excellent electrochemical performances are not systematic. In this paper, we will focus our eyes on Co3O4and a-Ni(OH)2. After consciously manipulating materials with3D hierarchical structures, electrochemical performances of them in supercapacitors are investigated systematically.
Co3O4micro hollow spheres are prepared using carbon spheres as templates through a one-pot hydrothermal carbonization and calcination method. Carbonization process of the precursor at a low hydrothermal temperature of140℃is investigated by FTIR and Raman spectra. Effects of the concentration of the starting materials and hydrothermal reaction time on the size and thickness of carbon spheres are studied. When calcined at500℃in air, Co3O4hollow spheres with high purity are obtained. The role of BET surface area and pore diameter of Co3O4on their electrochemical performances are discussed. Owing to the relative high surface area and moderate pore diameter, the Co3O4micro hollow spheres display higher specific capacitance and excellent cycle performance.
a-Ni(OH)2with different morphologies and BET surface areas are prepared through a solvothermal method using different alcohols and water as the mixing solvent. Effects of physical characters of alcohols on the morphologies of the product are studied. a-Ni(OH)2microspheres constructed by nanowires with a BET surface area of318.6m2g-1are obtained using triethylene glycol and water as the mixed solvent. Owing to the high BET surface area and large pore volume, this sample displays a high specific capacity of1788.9F g-1at a current density of0.5A g-1. Besides, rate performance of this sample is also excellent. This can be attributed to the small size of the nanowires constructing the microspheres, which can effectively shorten the proton diffusion distance and lower the ion diffusion resistance. Besides, the large BET surface area of the sample can ensure a sufficient contact between the active materials of the electrode and the electrolytes, making the chemically active materials almost100%usable for the redox reaction.
本文采用化学还原法制备了Co-Se复合物,并将其用作碱性二次电池负极材料。放电电流密度为50mAg-1时其放电容量高达380mAhg-1,且循环稳定性良好：130周后,放电容量依然达到356.5mAhg-1,放电容量保持率在93.62%。同等条件下Co电极的放电容量只有130mAhg-1。这主要是由于复合物中的Se提高了Co的分散性能,同时Se在电化学反应过程中逐渐溶解,使电极内产生空隙,增加了Co与电解液接触的面积,提高了电化学反应的效率,进而提高了Co的利用率。对Se在此过程中的作用和反应机理进行了深入探究。
采用物理球磨的方法制备Co-Se-C复合材料并将其用作镍基碱性二次电池负极材料。加入的Se和CNTs较大程度的提高了Co的放电容量,最大放电比容量达到450mAhg-1,同时材料的活化周期明显缩短。这主要是由于Se和CNTs的协同作用,Se的溶解增加了电极活性物质与电解液的接触；而CNTs的引入增加了材料的导电性和韧性。
Co304是一种P型半导体,且其中Co的价态较高,是一种潜在的多电子反应电极材料,我们预测它和CoO、Co(OH)2等一样,有望在镍基碱性二次电池中应用。
本文中采用溶解热和高温煅烧两步法制备了不同形貌的C0304,并将其用作碱性二次电池负极材料。在100mAg-1的电流密度下,多面体C0304最高放电容量能够达到399.9mAh g-1。继续采用降低前驱体煅烧温度的方法,使得材料的比表面积增大,最大放电容量提高至490.2mAhg-1,且循环稳定性良好。对CO3O4电极在充放电过程中的电化学反应机理进行了研究,发现C0304在充电过程中先转化成Co(OH)2,然后继续转化成Co。放电容量主要来源于Co(OH)2与Co的转化。
镍钴氧化物／氢氧化物等由于具有较高的理论放电比容量、价格低廉、电化学氧化还原可逆性好等优点成为较有前途的新型超级电容器材料,目前虽然相关报道较多,但是关于材料的特殊形貌制备和性能研究尚不成体系。本文将以Co3O4、α-Ni(OH)2材料作为研究对象,研究其作为超级电容器电极材料的电化学性能。
采用碳球模板法一步低温水热合成空心C0304微米球。系统研究了在140℃较低温度下前躯体的碳化过程。同时也考察了反应物浓度、反应时间等因素对碳球尺寸、厚度等的影响。采用500℃空气煅烧得到纯度较高的空心Co3O4微米球。研究了C0304的比表面积、孔径等对电化学性能的影响。由于材料具有较大的比表面积和较合适的孔径,在被用作电容器材料时显示了较高的比电容和优异的循环性能。
利用不同的醇和水作混合溶剂,采用溶剂热法制备了不同形貌和比表面积的α-Ni(OH)2。研究了醇的物理性质对材料形貌的影响。当用二缩三乙--醇和水做混合溶剂时,制备的纳米线堆积的α-Ni(OH)2微米球比表面积达到318.6m2g1。在未复合其他材料的情况下,其放电比容量达到1788.9F g-1(放电电流密度为0.5A g-1),且循环性能良好。这主要是由于组成材料的纳米线尺寸较小,这种结构有效缩短了质子扩散路径,离子扩散阻力也很大程度得到了降低。同时材料的比表面积很大,使得电解液能够渗入活性物质内部,活性物质有效接触面积增大,从而提高了电化学反应效率。
A series of Co-X materials, such as Co-B, Co-Si, Co-P, Co-S, Co-BN and so on, are reported to demonstrate high discharge capacity and excellent cycle stability in alkaline rechargeable batteries. The inactive part can dissolve in alkaline aqueous, resulting in the creation of newly built interspaces among the Co particles. These newly built interspaces can increase the contact area between the active electrode materials of the electrodes and alkaline electrolyte. Thus the efficiency of electrochemical reactions is enhanced, resulting in better electrochemical performance than pure Co. As we know, Selenium can also dissolve in alkaline solutions, which is similar with B, Si, P and S. Besides, the electric conductivity of selenium is better than the above-mentioned elements. It is expected that Se has similar functions in electrochemical application. However, report on its application in alkaline rechargeable batteries has not been found.
Co-Se composite is prepared through a chemical-reduction method and used as the negative electrode material of alkaline rechargeable batteries. The Co-Se composite shows a maximum discharge capacity of380mAh g-1at a current density of50mA g-1. After130cycles, the discharge capacity can still remain at356.5mAh g-1, with a retention rate of93.62%. As a comparison, the discharge capacity of pure Co is only130mAh g-1. This phenomenon can be explained as follows:the incorporation of Se improves the dispersibility of Co in the electrode. In addition, Se dissolves in the alkaline electrolytes, leading to more interspaces in the electrode, which is beneficial for increasing the contact area between the active materials and the electrolytes, thus enhances the efficiency of electrochemical reactions. Effect and function mechanism of Se in the electrochemical process are investigated in-depth.
Co-Se-C composite is prepared through ball-milling method and used as the negative electrode material of alkaline rechargeable batteries. The discharge capacity of Co is obviously improved after the incorporation of Se and CNTs. The maximum discharge capacity of it can reach450mAh g-1at the discharge current density of50 mA g-1. Besides, the cycle number needed to reach the maximum discharge capacity is decreased. This can be attributed to the synergetic effect of Se and CNTs. The dissolution of Se enhances the effective contact between the active material and the electrolytes; whereas the introduction of CNTs improves the conductivity and toughness of the material.
Co3O4is an important P-type semiconductor, in which the average valence of Co is8/3. So it is a potential multi-electron electrode material in alkaline rechargeable batteries. It is expected to display excellent performance as Co(OH)2and CoO.
Co3O4with different morphologies are prepared by a solvothermal/calcination method. Their electrochemical performances as electrode materials of alkaline rechargeable batteries are investigated. The maximum discharge capacity of Co3O4polyhedrons can reach399.9mAh g-1at the discharge current density of100mA g-1. By lowering the calcination temperature, the BET surface area of the sample is enlarged and the electrochemical discharge capacity is increased. The maximum discharge capacity reaches490.2mAh g-1. And the cycle performance is excellent. Reaction mechanism of Co3O4during electrochemical performance is discussed in detail. Co3O4first changes to Co(OH)2in the charged state and then to Co. Faradaic reaction between Co and Co(OH)2accounts for most of the discharge capacity.
Owing to their relative high specific capacitance, excellent reversible redox behavior and low cost, Cobalt/Nickel oxides and hydroxides have been considered as new types of supercapacitor electrode materials. Although many reports have been focused on them, preparation of materials with particular morphologies and excellent electrochemical performances are not systematic. In this paper, we will focus our eyes on Co3O4and a-Ni(OH)2. After consciously manipulating materials with3D hierarchical structures, electrochemical performances of them in supercapacitors are investigated systematically.
Co3O4micro hollow spheres are prepared using carbon spheres as templates through a one-pot hydrothermal carbonization and calcination method. Carbonization process of the precursor at a low hydrothermal temperature of140℃is investigated by FTIR and Raman spectra. Effects of the concentration of the starting materials and hydrothermal reaction time on the size and thickness of carbon spheres are studied. When calcined at500℃in air, Co3O4hollow spheres with high purity are obtained. The role of BET surface area and pore diameter of Co3O4on their electrochemical performances are discussed. Owing to the relative high surface area and moderate pore diameter, the Co3O4micro hollow spheres display higher specific capacitance and excellent cycle performance.
a-Ni(OH)2with different morphologies and BET surface areas are prepared through a solvothermal method using different alcohols and water as the mixing solvent. Effects of physical characters of alcohols on the morphologies of the product are studied. a-Ni(OH)2microspheres constructed by nanowires with a BET surface area of318.6m2g-1are obtained using triethylene glycol and water as the mixed solvent. Owing to the high BET surface area and large pore volume, this sample displays a high specific capacity of1788.9F g-1at a current density of0.5A g-1. Besides, rate performance of this sample is also excellent. This can be attributed to the small size of the nanowires constructing the microspheres, which can effectively shorten the proton diffusion distance and lower the ion diffusion resistance. Besides, the large BET surface area of the sample can ensure a sufficient contact between the active materials of the electrode and the electrolytes, making the chemically active materials almost100%usable for the redox reaction.
引文
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