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南昌大学彭洪根教授团队Nature Communications:一个催化剂覆盖280–600 °C:质子酸位点介导NH₃存储实现超300 °C活性温窗

  • 2026-07-16 04:01:24
南昌大学彭洪根教授团队Nature Communications:一个催化剂覆盖280–600 °C:质子酸位点介导NH₃存储实现超300 °C活性温窗
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第一作者:李国波 博士通讯作者:彭洪根 教授通讯单位:南昌大学资源与环境学院


研究背景:宽温域脱硝的“跷跷板”困境

氮氧化物(NOₓ)是雾霾和近地面臭氧的重要前体物,氨选择性催化还原(NH₃-SCR)是目前应用最广泛的固定源脱硝技术。然而,传统商用催化剂如V₂O₅-WO₃/TiO₂面临着一个根本性的性能瓶颈:操作温度窗口过窄

这一瓶颈源于一对难以调和的矛盾。NH₃-SCR反应需要催化剂同时完成两项任务——吸附并储存NH₃(需要酸性位点),以及活化反应分子完成氧化还原过程(需要氧化还原中心)。这两者之间存在类似跷跷板的关系:酸性过强会抑制氧化还原活性,氧化能力过强又会导致NH₃在高温下被过度氧化为NOₓ,反而增加排放。传统氧化物催化剂在这两者之间长期处于“顾此失彼”的窘境。

在钢铁烧结、水泥窑炉等非电力行业,烟气温度波动剧烈——从200 °C到500 °C以上的区间变化并不罕见。传统催化剂的窄温窗特征使其在低温时活性不足,在高温时又因NH₃过氧化而失效,严重制约了NH₃-SCR技术在这些行业的推广应用。


核心策略:让“储氨”和“反应”各司其职

彭洪根教授团队的核心思路,是用空间分工来打破性能跷跷板:将NH₃的储存功能和氧化还原功能分配给两种不同的材料,各自由最擅长的组分承担。

研究团队构建了一种“氧化物-分子筛”(OXZEO)耦合催化剂。在这一设计中:

  • 分子筛的孤立质子酸位点(B酸,≡Si–O(H)–Al≡) 充当“NH₃储库”。这些位点对NH₃具有强亲和力,能以NH₄⁺形式将氨分子捕获并稳定储存,且在高温下不易释放失控。
  • 复合金属氧化物担任氧化还原活性中心,负责活化NOₓ并催化还原反应。
  • 反应过程中,储存在分子筛中的NH₃以NH₃分子和NH₄⁺两种形式缓慢释放并迁移至氧化物表面参与反应。其中,NH₄⁺在高温环境下远较NH₃分子难以被氧化,从而从根本上抑制了高温段的NH₃过氧化副反应

这一“存储-迁移-反应”的模式,将传统催化剂中纠缠在一起的酸性和氧化还原功能在空间上解耦,让二者“各司其职、协同增效”。


机制解析:NH₄⁺如何成为高温段的“保护伞”

研究团队通过原位红外光谱、同位素标记-质谱联用、从头算分子动力学模拟及密度泛函理论计算,系统揭示了B酸位点介导的NH₃“存储-迁移”机制。

关键发现是:NH₃在分子筛中以NH₄⁺形式固定于B酸位点后,其在高温下的释放和迁移行为与游离态NH₃存在本质差异。 低温段,NH₃主要以分子形式脱附并迁移;而在高温段,部分NH₃以NH₄⁺形态直接穿梭至氧化物活性中心。由于NH₄⁺的N–H键断裂需要更高的活化能,它在到达氧化还原位点后不会立即被过度氧化为NO,而是按需参与SCR反应。

以CeSnOₓ/Beta为模型催化剂的测试结果显示,NOₓ转化率>80%的温度窗口从纯CeSnOₓ的320–500 °C大幅拓宽至280–600 °C——活性温窗跨度超过300 °C,且N₂选择性保持在99%以上。这一结果意味着,无论是在钢铁烧结烟气的中低温段(~250–350 °C)还是水泥窑尾气的高温段(~400–550 °C),同一催化剂均可保持高效稳定运行。


普适性验证:不止一种分子筛,不止一种氧化物

一项催化剂设计策略是否有生命力,取决于它能否跳出“一例一用”的特例范畴。

研究团队将该OXZEO设计原则推广至多种分子筛拓扑结构(BEA、CHA、MFI、FAU)及不同金属氧化物体系(Ce基、Mn基),所构建的催化剂均表现出显著拓宽的脱硝温度窗口。这一通用性说明,“质子酸位点储氨+氧化物活化反应”的分工逻辑具有跨材料体系的适用性,为宽温窗NH₃-SCR催化剂的理性设计确立了一条可复制、可推广的技术路线。


工程意义与展望

本研究为工业烟气脱硝提供了一条清晰的催化剂设计新范式。其核心价值在于,通过材料层面的功能解耦解决了一个困扰领域多年的“跷跷板”矛盾,且策略具有明确的普适性。对于我国钢铁、水泥等排放基数大、烟气工况复杂的非电行业,这一进展为开发适应性强、运行窗口宽的脱硝催化剂提供了理论指导与实验基础。


作者信息

李国波(第一作者):博士,南昌大学资源与环境学院。

彭洪根(通讯作者):教授,国家级青年人才,南昌大学资源与环境学院副院长、国家重点研发计划(青年)项目首席科学家。课题组长期致力于大气污染治理与温室气体资源化研究,聚焦NOₓ和VOCs的催化净化与资源化。


论文链接Zeolitic Isolated Protonic Acid Sites-Mediated NH₃ Storage for Robust NOₓ Removal. Nature Communications, 2026.https://www.nature.com/articles/s41467-026-75294-0

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  1. CONNECT:[ UseTime:0.000653s ] mysql:host=127.0.0.1;port=3306;dbname=aa460;charset=utf8mb4
  2. SHOW FULL COLUMNS FROM `fenlei` [ RunTime:0.000821s ]
  3. SELECT * FROM `fenlei` WHERE `fid` = 0 [ RunTime:0.000368s ]
  4. SELECT * FROM `fenlei` WHERE `fid` = 63 [ RunTime:0.000284s ]
  5. SHOW FULL COLUMNS FROM `set` [ RunTime:0.000485s ]
  6. SELECT * FROM `set` [ RunTime:0.000198s ]
  7. SHOW FULL COLUMNS FROM `article` [ RunTime:0.000577s ]
  8. SELECT * FROM `article` WHERE `id` = 539059 LIMIT 1 [ RunTime:0.023388s ]
  9. UPDATE `article` SET `lasttime` = 1784305873 WHERE `id` = 539059 [ RunTime:0.001520s ]
  10. SELECT * FROM `fenlei` WHERE `id` = 64 LIMIT 1 [ RunTime:0.000272s ]
  11. SELECT * FROM `article` WHERE `id` < 539059 ORDER BY `id` DESC LIMIT 1 [ RunTime:0.005234s ]
  12. SELECT * FROM `article` WHERE `id` > 539059 ORDER BY `id` ASC LIMIT 1 [ RunTime:0.000980s ]
  13. SELECT * FROM `article` WHERE `id` < 539059 ORDER BY `id` DESC LIMIT 10 [ RunTime:0.015180s ]
  14. SELECT * FROM `article` WHERE `id` < 539059 ORDER BY `id` DESC LIMIT 10,10 [ RunTime:0.000989s ]
  15. SELECT * FROM `article` WHERE `id` < 539059 ORDER BY `id` DESC LIMIT 20,10 [ RunTime:0.024561s ]
0.145623s