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南京大学,马年首篇Science!

  • 2026-03-18 19:56:15
南京大学,马年首篇Science!
时隔8个月，南京大学黎建团队再发《Science》：36元环超大孔沸石问世！
在石油化工和精细化工领域，大分子原料的高效转化始终受限于催化材料的孔径与稳定性。传统介孔分子筛虽具备较大孔道，却因无定形骨架而热稳定性不足；高硅沸石则结构稳定、酸性优异，却大多停留在微孔尺度，难以处理体积庞大的分子。如何在保持晶体结构稳定性的同时，实现真正“有序、可调、超大孔”的介孔沸石结构，成为国际催化材料领域的核心难题之一。
今日，南京大学黎建研究员联合苏州实验室徐乐研究员和中国石化石油化工研究院石油分子与过程工程国家重点实验室林伟研究员共同报道了一种全新高硅沸石NJU120-6。该材料首次实现由36元环构筑的本征圆柱形介孔通道，自由孔径高达25.71 Å × 19.12 Å，框架密度低至9.39 Si nm⁻³，孔体积达到0.66 cm³ g⁻¹，并在1173 K下仍保持结构稳定。同时，材料可引入Al和Ti等活性位点，在重油裂解和大分子环氧化反应中表现出优异催化性能，为大分子催化转化提供了全新平台。相关成果以A 36-ring zeolite with intrinsic cylindrical mesopores为题发表在《Science》上，孙嘉政和田旭东为共同第一作者。
值得一提的是，这是黎建研究员团队继2025年6月26日发表于《Science》之后的又一项重磅成果。
超大孔的“分子积木”设计
研究的突破首先源于结构导向剂（OSDA）的创新设计。如图1a所示，团队采用双膦鎓型大体积二阳离子分子，通过类似“乐高积木”的模块化拼接方式构建模板分子。这种刚性头基加柔性链段的bola型结构，为超大孔道的形成预留了充足空间。在其诱导下形成的NJU120-6框架如图1b所示，从[001]方向观察可见规则排列的巨大孔道。而图1c则直观展示了该材料的晶体学孔径：由36个硅原子围成的孔窗形成近圆柱形通道，自由直径达到25.71 Å × 19.12 Å。这一尺寸已正式跨入介孔区间，成为目前已报道沸石中最大的环孔结构之一。值得强调的是，与此前报道的ITQ-37、ITQ-43等拉长型孔道不同，NJU120-6的孔道截面更接近圆形，意味着大分子扩散更加顺畅，也更有利于实际催化过程中的传质效率。
图1：双膦鎓结构导向剂设计及NJU120-6的36元环超大孔结构示意图。
36元环如何“拼”出来？
如果说图1回答了“孔有多大”，那么图2则解释了“孔是怎么形成的”。图2a展示了构筑NJU120-6的四种基本笼结构单元，包括t-sgt、t-ewt与t-pes等不同拓扑构件。这些结构单元在ab平面交替连接，形成波浪状层结构；进一步沿c轴通过氧桥连接，构筑三维骨架。图2b中可以看到，由6个t-sgt、6个t-ewt以及6个组合笼结构构成一个超大复合结构单元，其中中心即形成36元环孔道（图2c）。这种高度对称且规则排列的超大孔道，在电子显微镜图像中得到了直接验证——图2d和2e的iDPC-STEM与ADF-STEM图像清晰显示出笔直贯通的36元环通道。此外，该材料框架密度仅9.39 Si nm⁻³，对应理论密度约0.956 g cm⁻³，甚至低于水。这意味着NJU120-6在保持晶体稳定性的同时，实现了极端开放的骨架结构，在所有已知四配位氧化物中属于最低密度序列之一。
图2：NJU120-6的拓扑结构单元拼接方式及36元环孔道的电子显微镜实证。
模板分子如何“卡位”？
结构的形成离不开有机模板的精准嵌入。图3a给出了Rietveld精修结果，实验数据与理论计算高度吻合，证明结构解析准确可靠。图3b进一步揭示了OSDA在36元环孔道内部的具体位置。可以看到，双膦鎓结构完整嵌入超大孔道中，其刚性头部固定在孔壁附近，而中间柔性链段跨越孔腔，恰好维持了圆柱形孔道空间。这种“撑开式”构型为超大孔的形成提供了稳定支撑。经600°C煅烧后，有机模板被去除，框架结构依然保持完整。氮气与氩气吸附实验显示其呈现典型IV型等温线，进一步确认其介孔特征。
图3：Rietveld精修结果及模板分子在36元环孔道中的空间分布。
从结构走向应用
真正决定材料价值的，是其催化表现。图4a与4b展示了NJU120-6的孔径分布与孔体积分析。吸附数据计算得到比表面积超过1300 m² g⁻¹，孔径峰值约2.6 nm，与晶体学孔径高度一致。在重油催化裂解实验中（图4c），含铝的Al-NJU120-6表现出优异的汽柴油选择性（约44.7%），气体副产物比例低，几乎不积炭。相比USY和Beta沸石，NJU120-6因其更大孔径与适中酸性，避免了过度裂解和焦炭快速生成的问题。在钛掺杂体系中（图4d），Ti-NJU120-6在环辛烯与TBHP氧化反应中表现出更高转化率与TON值，明显优于Ti-Beta和Ti-MCM-41。超大有序孔道显著提升了大分子底物的扩散与活性位点利用率。
图4：NJU120-6的孔结构分析及其在重油裂解和环氧化反应中的催化性能表现
小结
NJU120-6的诞生，标志着沸石材料在“稳定性”与“超大孔”之间实现真正兼得。通过双膦鎓模板分子的精准分子设计，团队成功构筑了首个由36元环定义的本征圆柱形介孔沸石，刷新了孔径纪录，并保持了高热稳定性与低框架密度。更重要的是，该材料不仅在结构层面实现突破，更在重油裂解与大分子氧化等工业关键反应中展现出现实应用潜力。随着更多异原子掺杂与功能化探索的推进，NJU120-6有望成为大分子催化转化领域的重要基础平台材料。
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  1. CONNECT:[ UseTime:0.000505s ] mysql:host=127.0.0.1;port=3306;dbname=b460;charset=utf8mb4
  2. SHOW FULL COLUMNS FROM `fenlei` [ RunTime:0.000732s ]
  3. SELECT * FROM `fenlei` WHERE `fid` = 0 [ RunTime:0.000326s ]
  4. SELECT * FROM `fenlei` WHERE `fid` = 63 [ RunTime:0.002577s ]
  5. SHOW FULL COLUMNS FROM `set` [ RunTime:0.000634s ]
  6. SELECT * FROM `set` [ RunTime:0.000217s ]
  7. SHOW FULL COLUMNS FROM `article` [ RunTime:0.000636s ]
  8. SELECT * FROM `article` WHERE `id` = 489008 LIMIT 1 [ RunTime:0.000458s ]
  9. UPDATE `article` SET `lasttime` = 1775439484 WHERE `id` = 489008 [ RunTime:0.000694s ]
  10. SELECT * FROM `fenlei` WHERE `id` = 65 LIMIT 1 [ RunTime:0.000236s ]
  11. SELECT * FROM `article` WHERE `id` < 489008 ORDER BY `id` DESC LIMIT 1 [ RunTime:0.000436s ]
  12. SELECT * FROM `article` WHERE `id` > 489008 ORDER BY `id` ASC LIMIT 1 [ RunTime:0.000358s ]
  13. SELECT * FROM `article` WHERE `id` < 489008 ORDER BY `id` DESC LIMIT 10 [ RunTime:0.003436s ]
  14. SELECT * FROM `article` WHERE `id` < 489008 ORDER BY `id` DESC LIMIT 10,10 [ RunTime:0.000681s ]
  15. SELECT * FROM `article` WHERE `id` < 489008 ORDER BY `id` DESC LIMIT 20,10 [ RunTime:0.001048s ]
0.086693s