Robust route to H(2)O(2) and H(2) via intermediate water splitting enabled by capitalizing on minimum vanadium-doped piezocatalysts.
Robust route to H(2)O(2) and H(2) via intermediate water splitting enabled by capitalizing on minimum vanadium-doped piezocatalysts.
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利用最少的钒掺杂压电催化剂，通过中间水分解生成 H2O2 和 H2
DOI：
10.1007/s12274-022-4506-0
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发表时间：
2022
期刊：
影响因子：
9.9
通讯作者：
中科院分区：
文献类型：
--
作者：
H2 O2是一种环境友好的化学品，用于各种水处理。工业生产H2 O2是蒽醌氧化法，但该方法消耗大量能源并产生污染。在这里，我们报告了一个绿色和可持续的压电催化中间水裂解过程，同时获得H2 O2和H2使用单晶钒（V）掺杂的铌酸钠（V-NaNbO 3）纳米立方体作为催化剂。V的引入提高了NaNbO 3的比表面积和活性位。值得注意的是，10 mg的V-NaNbO 3压电催化剂表现出比50 mg的相同催化剂高3.1倍的压电催化效率，因为更多的压电催化剂导致更高的聚集概率。由于不同纳米催化剂之间的中和作用，聚集导致活性位点减少，内建电场降低。值得注意的是，V-NaNbO 3（10 mol%）纳米立方体的压催化H2 O2和H2生产速率（分别为102.6和346.2 µmol·g−1·h−1）分别比制备的原始NaNbO 3对应物增加了2.2和4.6倍。通过压电响应力显微镜（PFM）和密度泛函理论（DFT）模拟发现，这种催化效率的提高是由于V掺杂后NaNbO 3催化剂的压电响应和更多的活性中心。更重要的是，我们的DFT结果表明，引入V可以降低水在NaNbO 3上解离的动力学势垒，从而提高H2 O2和H2的产率。这种简便而强大的压电催化路线使用最少量的催化剂，以获得H2 O2和H2可能脱颖而出，作为一个有前途的候选环境应用和水裂解。补充材料（不同掺杂浓度的NaNbO 3和V-NaNbO 3的典型拉曼光谱（图S1）。Na 1 s的XPS光谱（图S2）。从使用NaNbO 3和V-NaNbO 3（10摩尔%）作为催化剂的压电催化体系获得的溶液在1小时后的PL光谱（图S3）。NaNbO 3和V-NaNbO 3纳米立方体的长度根据其（101）面的XRD数据计算（表S1））可在本文的在线版本10.1007/s12274-022-4506-0中获得。
H2O2 is an environmentally friendly chemical for a wide range of water treatments. The industrial production of H2O2 is an anthraquinone oxidation process, which, however, consumes extensive energy and produces pollution. Here we report a green and sustainable piezocatalytic intermediate water splitting process to simultaneously obtain H2O2 and H2 using single crystal vanadium (V)-doped NaNbO3 (V-NaNbO3) nanocubes as catalysts. The introduction of V improves the specific surface area and active sites of NaNbO3. Notably, V-NaNbO3 piezocatalysts of 10 mg exhibit 3.1-fold higher piezocatalytic efficiency than the same catalysts of 50 mg, as more piezocatalysts lead to higher probability of aggregation. The aggregation causes reducing active sites and decreased built-in electric field due to the neutralization between different nano-catalysts. Remarkably, piezocatalytic H2O2 and H2 production rates of V-NaNbO3 (10 mol%) nanocubes (102.6 and 346.2 µmol·g−1·h−1, respectively) are increased by 2.2 and 4.6 times compared to the as-prepared pristine NaNbO3 counterparts, respectively. This improved catalytic efficiency is attributed to the promoted piezo-response and more active sites of NaNbO3 catalysts after V doping, as uncovered by piezo-response force microscopy (PFM) and density functional theory (DFT) simulation. More importantly, our DFT results illustrate that inducing V could reduce the dynamic barrier of water dissociation over NaNbO3, thus enhancing the yield of H2O2 and H2. This facile yet robust piezocatalytic route using minimal amounts of catalysts to obtain H2O2 and H2 may stand out as a promising candidate for environmental applications and water splitting. Supplementary material (typical Raman spectra of NaNbO3 and V-NaNbO3 with various doping concentrations (Fig. S1). XPS spectra of Na 1s (Fig. S2). PL spectra of solution obtained from the piezocatalytic system using NaNbO3 and V-NaNbO3 (10 mol%) as the catalysts after 1 h (Fig. S3). The length of NaNbO3 and V-NaNbO3 nanocubes calculated from XRD data of their (101) planes (Table S1)) is available in the online version of this article at 10.1007/s12274-022-4506-0.
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