Article(id=1320098198237073503, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320098188355285873, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20230782, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1696953600000, receivedDateStr=2023-10-11, revisedDate=1698422400000, revisedDateStr=2023-10-28, acceptedDate=null, acceptedDateStr=null, onlineDate=1792665536698, onlineDateStr=2026-10-22, pubDate=1726761600000, pubDateStr=2024-09-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792665536698, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792665536698, creator=13701087609, updateTime=1792665536698, updator=13701087609, issue=Issue{id=1320098188355285873, tenantId=1146029695717560320, journalId=1263187385517883426, year='2024', volume='52', issue='9', pageStart='2755', pageEnd='3090', issueExtLink='null', onlineDate='null', pubDate='1726761600000', pubDateStr='2024-09-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792665534341, creator='13701087609', updateTime=1792666312798, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320101453507711442, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320098188355285873, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320101453507711443, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320098188355285873, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=3027, endPage=3035, ext={EN=ArticleExt(id=1320098198434205792, articleId=1320098198237073503, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Photothermal Catalytic Reforming of Cellulose for Hydrogen Production with CuNi Alloylpalygorskite nanocomposites, columnId=1319726165087077079, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction Sustainable H2 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 H2. 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 CuCl2·2H2O and 0.1 mol Ni(NO3)2·6H2O 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 highest 36.8 μ mol · g-1 · h-1, followed by lactic acid 13.8 μmol·g-1·h-1. After the conversion of cellulose into glucose, the C—C bond in glucose finally breaks to generate formate. Compared with Cu/H-Pal and Ni/H-Pal, the CuNi/H-Pal hydrogen production efficiency is higher, because the synergistic action of bimetals can effectively promote charge separation, while retaining the LSPR effect of copper particles, thus achieving the photothermal cooperative catalysis, and the highest hydrogen evolution rate is 1.68 mmol·g-1·h-1.
In the aqueous solution, cellulose is first adsorbed on the surface of Pal rod crystals, and under light irradiation, photogenerated electrons reduce H+ to H2 in water at the reduction end of CuNi/H-Pal. Due to the plasmon resonance effect of CuNi, CuNi/H-Pal has a significant photothermal effect, and the activity of acidic sites on the catalyst is enhanced under the synergistic effect of photothermal interaction, which promotes the cleavage of cellulose β-1,4-glycosidic bond and hydrolysis to glucose. Subsequently, the resulting glucose is converted to C5 sugar and formic acid by hole oxidation, and C5 sugar is converted to C4 sugar and formic acid through the Ruff degradation mechanism, and all intermediates are further gradually converted to formic acid through the C1-C2 α-splitting process. At the same time, cellulose conversion products contain small amounts of lactic acid. Cu on the surface of the catalyst acts as a small amount of Lewis acid active site during the catalytic reaction, promoting the conversion of glucose to lactate under the joint action of holes.
Conclusions In summary, a new plasma-metal-alloy supported by clay mineral nanocomposite material was prepared. Different amounts of CuNi alloys were loaded on the surface of phosphorylated Pal, which not only retained the plasmon resonance effect of Cu element, but also improved its stability and inhibited its oxidation, and significantly improved the charge transfer efficiency due to the Schottky junction formed by the metal alloy and modified Pal. The hydrogen production rate with 30% CuNi/H-Pal catalyst could reach 1.68 mmol g-1·h-1 under simulated sunlight irradiation. At the same time, cellulose was converted into high value-added formic acid and lactic acid, and the yields reached 36.8 μmol·g-1·h-1 and 13.8 μmol·g-1·h-1, respectively. This work provides a new strategy for hydrogen production and the production of valuable biochemicals through biomass photocatalytic reforming.
, authors=Xuhua YE, Rongrong GAO, Binyan WANG, Meng WU, Chao YAO, Xiazhang LI, authorsList=Xuhua YE, Rongrong GAO, Binyan WANG, Meng WU, Chao YAO, Xiazhang LI, authorCompany=null, correspAuthors=Xiazhang LI, authorNote=
YE Xuhua (1979-), male, Ph.D., Associate Professor. E-mail: yxh@cczu.edu.cn
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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。
, authors=业绪华, 高镕榕, 王宾彦, 吴梦, 姚超, 李霞章, authorsList=业绪华, 高镕榕, 王宾彦, 吴梦, 姚超, 李霞章, authorCompany=null, correspAuthors=李霞章, authorNote=
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李霞章（1980—），男，博士，教授
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业绪华（1979—），男，博士，副研究员
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