等离激元CuNi合金/凹凸棒石复合材料制备及其光热催化纤维素重整产氢  

Photothermal Catalytic Reforming of Cellulose for Hydrogen Production with CuNi Alloylpalygorskite nanocomposites

作　　者：业绪华[1] 高镕榕 王宾彦 吴梦 姚超[1] 李霞章[1] YE Xuhua;GAO Rongrong;WANG Binyan;WU Meng;YAO Chao;LI Xiazhang(Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou University,Changzhou 213164,Jiangsu,China)

机构地区：[1]常州大学,江苏省绿色催化材料与技术重点实验室,江苏常州213164

出　　处：《硅酸盐学报》2024年第9期3027-3035,共9页Journal of The Chinese Ceramic Society

基　　金：国家自然科学基金(51674043);常州市国际科技合作项目(CZ20230018)。

摘　　要：太阳能驱动光催化产氢有望解决能源短缺和环境问题。利用可再生生物质或其衍生物作为光催化过程中的空穴牺牲剂,不仅可以降低水分解中析氧反应的热力学势垒,动力学上有利于加速氢气的生成,而且可将生物质转化为高价值的化学品。本工作制备了一种非贵等离子体CuNi合金/凹凸棒石(Pal)纳米复合材料用于纤维素的光催化转化,发现凹凸棒石的胶体特性利于纤维素的吸附富集,CuNi合金由于2种金属之间的协同作用不仅保留了铜单质的等离子共振效应,而且可以提高稳定性和抑制氧化;CuNi合金与磷酸酸化的凹凸棒石(H-Pal)形成的肖特基结提供了电荷转移通道,提高了电荷转移效率,促进了电子空穴分离。等离子共振产生的热效应与H-Pal表面酸性位点协同作用,提供了丰富的活性位点,提高了纤维素的转化率和H2的生成率。当CuNi合金负载量为30%(质量分数)时,产氢效率最高,达到了1.67 mmol·g^(-1)·h^(-1),与此同时纤维素转化为高附加值甲酸和乳酸。Introduction Sustainable H_(2)generation from water splitting by solar-driven photocatalysis has been proposed as a promising alternative to increasingly reduced fossil fuels.However,such techniques still face great challenges in dynamics and thermodynamics.Biomass as a hole sacrificial agent is conducive to the generation of H_(2).Local surface plasmon resonance(LSPR)can effectively use solar energy and convert it into high-energy"hot carriers",and realize high efficiency solar energy to chemical energy conversion.Copper alloy inherits the LSPR effect of copper particles.Palygorskite(Pal)is a natural hydrated magnesium silicate mineral with large surface area and certain acid sites.In this work,Pal-loaded plasma alloy nanocomposite was prepared for photocatalytic reforming cellulose for synergistic hydrogen production.The phosphate group-modified Pal provides a large number of acidic sites for cellulose hydrolysis and glucose.At the same time,the LSPR effect of CuNi alloy increases the reaction temperature,realizes the photothermal cooperative catalysis,and further enhances the catalyst activity.Methods 2 g Pal was evenly dispersed in 100 ml phosphate solution,then the mixture was stirred in an 80℃water bath for 12 h.Thereafter,they were washed with deionized water and dried at 80℃for 16 h to obtain H-Pal.0.1 mol of CuCl_(2)·2H_(2)O and 0.1 mol Ni(NO_(3))_(2)·6H_(2)O were dissolved in 30 ml of sodium hydroxide solution,and various-Pal was added with 0.5 g ethylenediamine by stirring.About 1 mol of sodium phosphates was added to the solution,and the mixture was transferred to the reaction kettle,reacted at 180℃for 90 min,and then naturally cooled to room temperature.After washing,CuNi/H-Pal composite was obtained after vacuum drying for 6 h.Results and diScussion The photocatalytic reforming cellulose was produced under simulated sunlight.The conversion of cellulose reached a maximum of 82%for 30%CuNi/H-Pal.In the end product of photoreforming cellulose,the content of formic acid dominated,reaching the hi

关 键 词：凹凸棒石 铜镍合金 等离激元 光热催化 生物质产氢 

分 类 号：TB332[一般工业技术—材料科学与工程]