Baoyu Gao

Bio: Baoyu Gao is an academic researcher from Shandong University. The author has contributed to research in topics: Adsorption & Flocculation. The author has an hindex of 73, co-authored 662 publications receiving 22467 citations.

Single-atom catalysis in advanced oxidation processes for environmental remediation.

Abstract: Emerging single atom catalysts (SACs), especially carbon-based SACs are appealing materials in environmental catalysis because of their ultrahigh performances, environmental friendliness, structural/chemical robustness, and the maximum utilization of active metal sites. The metal centres, carbon matrixes, and coordination characteristics collectively determine the electronic features of carbon-based SACs, and their behaviours in catalysing peroxide activation and efficiencies in advanced oxidation processes (AOPs). However, there is lack of a comprehensive and critical review reporting the successful marriage of carbon-based SACs in AOP-based remediation technologies. It is particularly necessary to systematically compare and reveal the catalytic sites and the associated mechanisms of carbon-based SACs in diverse AOP systems. In this review, we highlight the synthetic strategies, characterisation, and computation of carbon-based SACs, and for the first time, showcase their innovative applications in AOP technologies. We unveil the origins of versatile catalytic oxidation pathways in different AOP systems and the mechanisms of micropollutant degradation over carbon-based SACs, distinguished from the upsized counterparts (metals/oxides and carbon substrates). We also provide directions to the rational design of on-demand SACs for green chemistry and environmental sustainability. Also, we suggest a designated and integrated experimental/theoretical protocol for revealing the structure-catalysis relations of SACs in AOP applications, and propose the prospects for future opportunities and challenges.

In-situ pyrolysis of Enteromorpha as carbocatalyst for catalytic removal of organic contaminants: Considering the intrinsic N/Fe in Enteromorpha and non-radical reaction

Abstract: An environmentally friendly, facile, and economical Fe/N co-doped carbonaceous material (Fe-N@C) was prepared by the in-situ pyrolysis of Fe/N rich Enteromorpha biomass for peroxymonosulfate activation and organic contaminants degradation. Results indicated that Enteromorpha-based catalysts prepared at high pyrolysis temperature displayed some highly graphitic nanosheets with rich nitrogen doped. The graphitic N derived from the intrinsic N in Enteromorpha showed the high correlation with the paracetamol (PCM) removal rate; this was confirmed by the Density Functional Theory (DFT) calculation, showing the high adsorption energy (ΔEads, −2.62 eV) of PMS molecular adsorbed onto the graphitic N area. A weak correlation between the PCM removal rate and adsorption capacity was also observed, revealing that the PCM catalytic reaction could be greatly accelerated after the pre-adsorption. It was interesting that the intrinsic Fe in Enteromorpha did not affect the PCM degradation, but PCM removal rate of acid treated Fe-N/C was improved as more active sites were formed after the Fe extraction by acid treatment. Both the radical pathways of O2 − and non-radical 1O2 generated in the Fe-N@C/PMS system were the primary mechanisms for the PCM degradation, which was consistent with the Fukui function values of f° and f- based on the DFT calculation. In addition, high stability of the carbon-based catalysts was observed after three runs and calcinating regeneration, which showed the promising applications for environmental remediation.

Sulfate saturated biosorbent-derived Co-S@NC nanoarchitecture as an efficient catalyst for peroxymonosulfate activation

Abstract: Using sulfate saturated bio-sorbent and cobalt(II) acetate as precursors, the homogeneous assembly of S-Co3O4 in nitrogen doped carbon martix (Co-S@NC) was obtained for the first time in an one-step pyrolysis. The reactions between peroxymonosulfate (PMS) and Co-S@NC for dinotefuran (DIN) decomposition were investigated. Co3O4 in Co@NC were primarily coordinated with the pyridinic N as catalytic sites. The adsorbed sulfate as S dopant was incorporated into the Co3O4 in carbon matrix due to the role of N as anchors, and the DIN decomposition of S-doped samples increased by 1.71 times as compared to the S-free sample (Co@NC). S incorporation can promote the formation of non-radical 1O2 and various radicals. In addition, DFT calculations indicated the enhanced electronic conductivity after S incorporation, which would facilitate the DIN decomposition in Co-S@NC/PMS system. This work enables the first insight into the role of adsorbed sulfate as effective S dopant for PMS activation.