<th id="5nh9l"></th><strike id="5nh9l"></strike><th id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"></th><strike id="5nh9l"></strike>
<progress id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"><noframes id="5nh9l">
<th id="5nh9l"></th> <strike id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"></span>
<progress id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"></span><strike id="5nh9l"><noframes id="5nh9l"><strike id="5nh9l"></strike>
<span id="5nh9l"><noframes id="5nh9l">
<span id="5nh9l"><noframes id="5nh9l">
<span id="5nh9l"></span><span id="5nh9l"><video id="5nh9l"></video></span>
<th id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"></th>
<progress id="5nh9l"><noframes id="5nh9l">

負載型Ru/CN催化劑的制備及其催化氨硼烷水解制氫

Preparation of supported Ru/CN catalysts and their performance in hydrogen generation from the catalytic hydrolysis of ammonia borane

  • 摘要: 氫的質量分數為19.6%的氨硼烷(AB)被廣泛認為是安全有效的氫氣儲存和釋放介質. 氮化碳(CN)材料由于其獨特的能帶結構、優良的化學穩定性以及N原子和C原子的配位框架,是AB水解催化劑的重要載體. 以三聚氰胺、三聚氰酸以及檸檬酸為原料高溫焙燒合成氮化碳載體(CN),再采用浸漬–還原法制備得到Ru/CN負載型納米催化劑. 利用各種表征手段來探究催化劑的結構組成及微觀形貌,進而考察不同因素對氨硼烷(NH3BH3,AB)水解制氫反應速率的影響. 結果表明:催化劑的晶格條紋間距為0.211 nm,對應于Ru的(002)晶面,證明Ru納米粒子成功負載于CN載體表面. Ru負載量為0.05 mmol的Ru/CN催化劑初始轉化頻率(TOF)為446.4 min–1,Ru/CN催化AB水解制氫反應相對于催化劑用量可以近似看作一級反應;升溫可以增大反應物分子之間的有效碰撞頻率,促使制氫反應更易進行;且經計算分析表明,AB濃度對于Ru/CN催化AB水解制氫反應具有正向影響,活化能為53.6 kJ·mol–1,Ru/CN催化劑在經過5次循環使用后,仍能催化AB完全水解制氫. 這項工作提出了一種構建含貴金屬的AB水解催化劑的有效方法.

     

    Abstract: Ammonia borane (AB) has a hydrogen mass fraction of 19.6% and is widely regarded as a safe and efficient medium for hydrogen storage and release. However, developing an effective catalyst to drive hydrogen evolution via AB hydrolysis remains a significant challenge. Carbon nitride (CN) materials exhibit a distinctive band structure, outstanding chemical stability, and a coordination framework composed of nitrogen and carbon atoms. The lone electron pairs on nitrogen atoms enhance their coordination with metal atoms more readily than those on carbon atoms. Consequently, most metal atoms preferentially coordinate with nitrogen, making CN a valuable support material for stabilizing noble-metal catalysts. Research indicates that noble metal catalysts, including ruthenium (Ru), silver, palladium, platinum, and rhodium, exhibit exceptionally high catalytic activity in hydrogen production via AB hydrolysis. Among these, Ru-based catalysts demonstrate superior performance in AB hydrolysis and are relatively more cost-effective than other noble metal-based catalysts. However, Ru nanoparticles are prone to agglomeration, highlighting the need for suitable support materials to mitigate this issue and enhance their stability. In this study, CN was synthesized via high-temperature calcination using melamine, cyanuric acid, and citric acid as raw materials. Subsequently, a Ru/CN-supported nanocatalyst was prepared via an impregnation-reduction method. Various characterization techniques were used to analyze the structural composition and microstructure of the catalysts. Additionally, the effects of different factors on the hydrogen production rate during the hydrolysis of ammonia borane (NH3BH3, AB) were systematically investigated. The results revealed that the Ru/CN catalyst exhibits an irregular morphology with a rough surface and depressions, which enhance its surface area and facilitate the formation of active metal sites. The lattice stripe spacing of 0.211 nm corresponds to the (002) crystal plane of Ru, confirming the successful loading of Ru nanoparticles onto the CN support. Furthermore, the Ru nanoparticles were highly dispersed on the support surface, providing abundant active sites for the hydrolytic dehydrogenation reaction of AB. The X-ray photoelectron spectroscopy full spectrum of the Ru/CN catalyst displayed distinct characteristic peaks for carbon (C), nitrogen (N), oxygen (O), and Ru, further verifying the successful incorporation of Ru onto the CN support. The detection of elemental Ru confirmed the successful reduction of Ru3+ by sodium borohydride. The presence of Ru in a higher oxidation state is likely due to the partial oxidation of elemental Ru during characterization or performance testing. The Ru/CN catalyst, with a Ru loading of 0.05 mmol, achieved a TOF value of 446.4 min–1. The AB hydrolysis hydrogen production reaction catalyzed by Ru/CN can be approximated as a first-order reaction with respect to the catalyst amount. Increasing the reaction temperature enhances the effective collision frequency between reactant molecules, thereby facilitating hydrogen production. Calculations and analyses revealed that the concentration of AB positively influences the Ru/CN-catalyzed reaction, with an activation energy of 53.6 kJ·mol–1. After five cycles of use, the Ru/CN catalyst remains effective in catalyzing the complete hydrolysis of AB for hydrogen production. This study offers a promising pathway for designing efficient noble-metal catalysts for AB hydrolysis.

     

/

返回文章
返回
<th id="5nh9l"></th><strike id="5nh9l"></strike><th id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"></th><strike id="5nh9l"></strike>
<progress id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"><noframes id="5nh9l">
<th id="5nh9l"></th> <strike id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"></span>
<progress id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"><noframes id="5nh9l"><span id="5nh9l"></span><strike id="5nh9l"><noframes id="5nh9l"><strike id="5nh9l"></strike>
<span id="5nh9l"><noframes id="5nh9l">
<span id="5nh9l"><noframes id="5nh9l">
<span id="5nh9l"></span><span id="5nh9l"><video id="5nh9l"></video></span>
<th id="5nh9l"><noframes id="5nh9l"><th id="5nh9l"></th>
<progress id="5nh9l"><noframes id="5nh9l">
259luxu-164