Single Atom Embedding Enhanced Macroscopic Polarization in Carbon Nitride Nanosheets for pH-Universal Piezo-Photocatalytic Nitrate Reduction over a Wide Concentration Range

作者：Jinzhou Liu, Lujie Jin, Zhongqin Dai, Yujin Ji, Jin Qian, Yan Lu, Jiong Wang, Bo Shen, Youyong Li, Rong Xu, Guanyu Liu, Jiwei Zhai · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.4c06247 · 被引用次数：48 · 研究领域：Advanced Photocatalysis Techniques、Advanced biosensing and bioanalysis techniques、Nanocluster Synthesis and Applications

Piezo-photocatalytic nitrate reduction reaction (NO 3 – RR) is an ammonia synthesis approach as a promising alternative to the conventional energy-intensive Haber–Bosch process. Herein, we designed carbon nitride nanosheet supported Cu single atom (C 3 N 4 /Cu) catalysts with tunable electronic structures via coordination environment engineering. The embedding of single atoms into carbon nitride leads to enhanced piezoelectricity, which originates from the induced non-centrosymmetric cavities in nanosheets. The resulting macroscopic polarization facilitates the transport of photogenerated charge carriers together with suppressed charge recombination endowed by rich nitrogen vacancies in C 3 N 4 /Cu. Furthermore, it favors the dissociation of water to provide sufficient active hydrogen for the hydrogenation of NO 3 – with reduced energy barriers during the NO 3 – RR. Consequently, C 3 N 4 /Cu attains an ammonia yield rate of up to 25.2 mg h –1 g cat –1 without a sacrificial reagent. Moreover impressively, it maintains yield rates above 5 mg h –1 g cat –1 at pH values of 1–14 and over a wide range of NO 3 – concentrations from 0.01 to 2 mol L –1, indicative of its catalytic versatility for actual wastewater treatment.