| 自支撑Cu/α-FeOOH/泡沫镍复合催化剂氧化甲醇耦合电解水高效制氢 | |
| Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis | |
| 摘要: 采用一步溶剂热法在泡沫镍(NF)基底上原位生长 Cu/α-FeOOH 纳米复合材料，制备了自支撑 Cu/α-FeOOH/NF 催化剂。相比于 α-FeOOH/NF催化剂，Cu的引入为 α-FeOOH的生长提供了更多的附着点，使得催化剂表面更加粗糙，并增大了催化剂与反应物的接触面积。Cu和无定形的 α-FeOOH 之间存在晶态和非晶态的异质界面，改变了催化剂的电子结构，促进电子从Ni、Fe向Cu转移，从而显著增强了催化剂对甲醇的吸附和氧化。电化学测试表明，Cu/α-FeOOH/NF催化剂具有优异的甲醇氧化反应(MOR)和析氢反应(HER)性能。在 Cu/α-FeOOH/NF 催化剂同时作为阴极、阳极的 Cu/α-FeOOH/NF||Cu/α-FeOOH/NFHER-MOR 耦合电解水系统中，达到 10 mA·cm-2电流密度所需的电压比直接全水解系统降低了 125 mV，且在较大电压(2.4 V)下能够稳定反应96 h。此外，阳极MOR产生了价值更高的甲酸盐，1.80 V下生成甲酸盐的法拉第效率高达97%。 | |
| 关键词: 甲醇氧化反应 异质界面 自支撑双功能催化剂 甲酸盐 耦合电解水制氢 | |
| 基金项目: 国家自然科学基金(No.22172143)资助。 | |
| Abstract: Self-supporting Cu/α-FeOOH/NF catalysts were prepared by in-situ growth of Cu/α-FeOOH nanocomposites on foam nickel (NF) substrate by one-step solvothermal method. Compared with the α-FeOOH/NF catalyst, adding Cu provided more attachment sites for the growth of α-FeOOH, which makes the catalyst surface morphology rougher and increases the contact area between the catalyst and reactants. The assembled heterointerface between crystalline Cu and amorphous α-FeOOH altered the electronic structure of the catalyst. It promoted electron transfer from Ni and Fe to Cu, thus enhancing methanol adsorption and oxidation. The electrochemical tests revealed that the Cu/α-FeOOH/NF catalyst exhibited excellent methanol oxidation reaction (MOR) and hydrogen evolution reaction (HER) performance. In the Cu/α-FeOOH/NF||Cu/α-FeOOH/NF HER-MOR system, the voltage was reduced by 125 mV compared to the overall water splitting system at the geometric current density of 10 mA·cm-2. The catalytic system operated stably for 96 h under high voltage (2.4 V). In addition, the anode MOR produced value-added formate and the calculated Faraday efficiency based on formate was close to 97% under an applied voltage of 1.80 V. | |
| Keywords: methanol oxidation reaction heterogeneous interface self-supporting bifunctional catalyst formate coupling electrolysis of water for hydrogen production | |
| 投稿时间：2024-01-21 修订日期：2024-08-30 | |
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| 申晴晴,杜向博文,钱凯成,金智康,方政,韦童,李仁宏.自支撑Cu/α-FeOOH/泡沫镍复合催化剂氧化甲醇耦合电解水高效制氢[J].无机化学学报,2024,40(10):1953-1964. | |
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