JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Huiwang Dai,Wenjun Zhou,Wei Wang,Zhiqi Liu
In this study, three Co/N-C catalysts were prepared by pyrolysis of bimetallic zeolitic imidazole frameworks with different Co/Zn ratio, and the critical active Co species in peroxymonosulfate (PMS) activation was investigated. The three catalysts had distinct cobalt species but similar N configuration and graphitization degree. The Co species were distributed as single atoms (Co SAs) at a Co/Zn molar ratio of 1:8, while Co nanoclusters (Co NCs) and Co nanoparticles (NPs) would be formed with further increase in Co content. The degradation efficiency of BPA did not show correlation with the increasing of Co content in catalyst. Based on the catalytic performance comparison and reactive species detection, Co SAs was identified as active sites, which could interact with PMS to generate 1 O 2 via path of PMS→HOO*→O*→ 1 O 2 . However, the role of NCs and NPs in directly activating PMS was negligible. In addition, the increase of Co content in Co/N-C catalyst would result in mass cobalt leaching, which enhanced the BPA degradation via homogeneous catalytic reactions with Co IV as reactive species. It is an effective way to design the Co/N-C catalyst with high catalytic activity and stability via regulating the formation of Co SAs.
研究领域:
环境化学
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催化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 8
·e202303088
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IF 1.9
Xiayan Zhang,Zhi Song,Boxia Liu,Jialu Liu,Yeqiong Huang,Dongxu Han
Graphical Ni/Fe bimetallic atom cluster catalyst is prepared by a hydrothermal to stimulate PMS to produce high concentration 1 O 2 and efficiently remove BPA from aqueous solution. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. The advanced oxidation process based on peroxymonosulfate (PMS) is a new water purification strategy. In this work, Ni/Fe bimetallic atom cluster composite catalyst is prepared by a hydrothermal synthesis to stimulate PMS to produce high concentration singlet oxygen ( 1 O 2 ) and efficiently remove bisphenol A (BPA) from aqueous solution. The experimental data show that in a broad pH range (pH=3–11), the removal rate of BPA by the non-free radical pathway induced by 1 O 2 is close to 100 %, and the catalyst still has high stability after 5 cycles. The mechanism of BPA removal in NiFe−BC/PMS/BPA catalytic degradation system is investigated by quenching experiment. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. In this paper, the high catalytic activity and selectivity of bimetallic atomic cluster catalysts can provide new insights for the treatment of phenolic wastewater.
研究领域:
环境科学
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催化
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水处理
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·2982-2994
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IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
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2023
·Vol. 52
·期 6
·1595-1601
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IF 4
Ziwei Wang,Lijuan Li,Weijin Wang,Runlin Wang,Guangzhe Li,Hang Bian,Dongxia Zhu,Martin R. Bryce
Cyclometalated Ir(III) complexes as photosensitizers (PSs) have attracted widespread attention because of their good photostability and efficient 1O2 production ability. However, their strong absorption in the UV-vis region severely limits their applications in photodynamic therapy (PDT) because the short wavelength illuminating light can be easily absorbed by the skin and subcutaneous adipose tissue causing damage to the patient's normal tissue. Herein, mono- and tetra-nuclear Ir(III) complex-porphyrin conjugates are rationally designed and synthesized, especially [TPP-4Ir]4+ exhibits obvious aggregation-induced emission (AIE) characteristics. PSs comprising Ir(III) complex-porphyrin conjugates self-assembled as nanoparticles (NPs) are successfully achieved. The obtained [TPP-Ir]+ NPs and [TPP-4Ir]4+ NPs exhibit long wavelength absorption (500–700 nm) and near-infrared emission (635–750 nm), successfully overcoming the inherent defects of short wavelength absorption of traditional Ir(III) complexes. Moreover, [TPP-4Ir]4+ NPs exhibit good biocompatibility, high 1O2 generation ability, low half-maximal inhibitory concentration (IC50) (0.47 × 10−6 M), potent cytotoxicity toward cancer cells and superior cellular uptake under white light irradiation. This work extends the scope for transition metal complex PSs with promising clinical applications.
研究领域:
材料科学
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纳米技术
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光动力疗法
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癌症研究
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光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）