用 ppm 级 Pd 对 WO3 进行氢溢出加速选择性加氢,ACS Applied Materials & Interfaces

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用 ppm 级 Pd 对 WO3 进行氢溢出加速选择性加氢
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-11 , DOI: 10.1021/acsami.3c00456
Yu Sun _{1,

2} , Bing Du ₃ , You Wang ₁ , Mingkai Zhang ₁ , Sai Zhang _{1,

2}

Affiliation

从金属到载体的氢溢出为设计用于选择性加氢的双活性位点催化剂开辟了一条新途径。然而，揭示氢溢出能力与加氢催化性能之间关系的知识非常有限。_{在此，已在 WO 3}负载的 ppm 级 Pd (PdHD/WO ₃ )上证明了依赖于氢溢出的选择性氢化，其中从 Pd 生成并溢出到 WO ₃的 *H 物质很容易用于添加反应物。具有六方相的WO ₃载体和合适的氧缺陷浓度可以增强氢溢出的能力，显着加速PdHD/WO _{3的催化活性}. 对于 4-氯硝基苯的加氢，具有最高氢溢出能力的PdHD/WO _{3催化剂产生了 47,488 h}^–1的周转频率 (TOF) （比传统 Pd/C 高 33 倍）。同时，得益于氢气溢出，4-氯硝基苯通过WO ₃氧空位上的硝基的独特吸附，保证了整个加氢过程中4-氯苯胺的选择性>99.9%。因此，这项工作有助于创造一种有效的方法来制造具有极低钯负载的具有成本效益的纳米催化剂，以实现具有极高活性和选择性的理想氢化。

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Hydrogen Spillover-Accelerated Selective Hydrogenation on WO3 with ppm-Level Pd

Hydrogen spillover from the metal to the support opens a fresh avenue to design dual-active site catalysts for selective hydrogenation. However, very limited knowledge has been obtained to reveal the relationship between the capacity of hydrogen spillover and catalytic performance of hydrogenation. Herein, hydrogen spillover-dependent selective hydrogenation has been demonstrated on WO₃-supported ppm-level Pd (PdHD/WO₃), where the *H species generated and spilled from Pd to WO₃ are readily utilized for addition of a reactant. The WO₃ supports with a hexagonal phase and a suitable oxygen defect concentration can enhance the capacity of hydrogen spillover, significantly accelerating the catalytic activity of PdHD/WO₃. For the hydrogenation of 4-chloronitrobenzene, the PdHD/WO₃ catalysts with the highest capacity of hydrogen spillover yielded a turnover frequency (TOF) of 47,488 h^–1 (33 times higher than that of traditional Pd/C). Meanwhile, benefiting from the hydrogen spillover, the unique adsorption of 4-chloronitrobenzene via the nitro group on the oxygen vacancy of WO₃ guaranteed >99.9% selectivity of 4-chloroaniline during the whole hydrogenation. This work thus helps to create an effective method for fabricating cost-effective nanocatalysts with an extremely low Pd loading for the ideal hydrogenation with extremely high activity and selectivity.

更新日期：2023-04-11

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