Jindi Yang, Hanqing Yin, Aijun Du, Mike Tebyetekerwa, Chuanbiao Bie, Zhuyuan Wang, Zhimeng Sun, Zhongguo Zhang, Xiangkang Zeng, Xiwang Zhang
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引用次数: 0
摘要
光催化氧还原反应（ORR）为过氧化氢（HO）的可持续生产提供了一种前景广阔的途径，但在开发具有良好 ORR 选择性的催化剂方面却面临着挑战。在此，我们报告了在非金属活性位点上定制 O 吸附可以优化 ORR 选择性。这一概念在三种具有不同原子构型的氮化碳上得到了验证：聚合氮化碳（PCN）、聚三嗪亚胺锂（Li-PTI）和聚庚嗪亚胺钠（Na-PHI）。对合成的 Na-PHI、PCN 和 Li-PTI 进行了表征，Na-PHI 在双电子 ORR 方面表现出卓越的光吸收、电荷载流子分离和显著的选择性（92%）。因此，Na-PHI 的 HO 生成率高达 3.48 mmol g h，分别是 Li-PTI 和 PCN 的 9.2 倍和 33 倍。这项研究强调了非金属活性位点吸附 O 对于选择性光催化 HO 生成的重要性。
Unveiling O2 adsorption on non-metallic active site for selective photocatalytic H2O2 production
Photocatalytic oxygen reduction reaction (ORR) offers a promising pathway for sustainable hydrogen peroxide (HO) production but faces challenges in developing catalysts with good ORR selectivity. Herein, we report that tailoring O adsorption on non-metallic active sites can optimize ORR selectivity. This concept is demonstrated on three carbon nitrides with different atomic configurations: polymeric carbon nitride (PCN), lithium-poly triazine imide (Li-PTI), and sodium-poly heptazine imide (Na-PHI). Na-PHI emerges as a strong candidate for HO production due to the end-on adsorption mode and suitable adsorption strength with O. Synthesized Na-PHI, PCN, and Li-PTI are characterized, with Na-PHI showing superior light absorption, charge carrier separation, and remarkable selectivity (92 %) for two-electron ORR. Consequently, Na-PHI achieves a high HO generation rate of 3.48 mmol g h, surpassing Li-PTI and PCN by 9.2 and 33 times, respectively. This study underscores the importance of O adsorption on non-metallic active sites for selective photocatalytic HO generation.
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