Effective removal of pollutants that affect human health and ecosystem stability is a crucial challenge. Here, the structural confinement engineering strategy realizes the effective anchoring of atomically dispersed Co in the B-doped-CN network (BCN) (BCN/CoN[2 +2]). The advanced oxidation process (AOP) involved BCN/CoN[2 + 2] has realized the rapid and complete degradation to tetracycline (TCL), the removal of approximately 80% and 100% of tetracycline was achieved in 5 min and 30 min, respectively. The AOP with BCN/CoN[2 + 2] can degrade TCL over a wide pH; in addition, BCN/CoN[2 + 2] has the ability to efficiently degrade common pollutants, and its catalytic activity did not decay even if it was used repeated five times. Electron paramagnetic resonance (EPR) spectroscopy shows that BCN/CoN[2 + 2] drives the complete conversion of peroxymonosulfate (PMS) to 1 O 2 , and density functional theory calculations demonstrate that the base for the conversion of PMS to 1 O 2 is from the isolated state of the active site Co.
Xue Zhao,Zhu Zhu,Yingnan He,Haibo Zhang,Xiaohai Zhou,Wanbiao Hu,Meng Li,Shusheng Zhang,Yemin Dong,Xun Hu,Artem V. Kuklin,Glib V. Baryshnikov,Hans Ågren,Thomas Wågberg,Guangzhi Hu
Electrochemical synthesis of ammonia driven by clean energy is expected to realize the supply of ammonia for distributed production of industry and agriculture. Here, nickel nanoparticles and nickel in the form of single atoms were simultaneously anchored on the electrochemically active carrier BCN matrix through a structured domain strategy, which realized a high-efficiency, high-value-added, conversion of nitrate in sewage. Specifically, the electrochemical nitrate reduction reaction (NIRR) driven by BCN@Ni in alkaline media achieves an ammonia yield rate as high as 2320.2 μg h −1 cm −2 (at −0.5 V vs RHE), and Faraday efficiency as high as 91.15% (at −0.3 V vs RHE). Even in neutral and acidic media, the ammonia yield rates of NIRR driven by BCN@Ni are as high as 1904.2 μg h −1 cm −2 and 2057.4 μg h −1 cm −2 , respectively (at −0.4 V vs RHE). The 15 NO 3 - isotope labeling experiment verified that the recorded ammonia all came from the electrochemical reduction of NO 3 – on BCN@Ni. Density functional theory (DFT) calculations show that both nano-Ni and single-atom Ni in BCN@Ni have the ability to electrochemically convert NO 3 – into NH 3 , and that the addition of BCN can further promote the NIRR on Ni.
危险品化学品经营许可证（带存储）