APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Bolong Zhao,Yulong Ma,Yonggang Sun,Guangsuo Yu,Juan Zhang,Li Zhu,Min Xu,Lei Wang,Duoning Zhao,Wenxin Ji,Yuanyuan Li,Yongsheng Ren
The traditional H 2 O 2 oxidation treating high-salt industrial wastewater is confronted with challenges, because of the inhibition of Cl - on oxidant radical. Thus, a non-radical pathway for H 2 O 2 removal of organic pollutants is optional. Herein, an innovative cobalt nitrogen-doped carbon (Co-N 5 -C) catalyst was constructed with an atomically dispersed asymmetrical high-density of Co-N 5 sites and highly active intermediate Co-OH groups, achieving highly selective converting H 2 O 2 to 1 O 2 through three steps electron transfer pathways. The oxidation of tetracycline by ¹O₂ accounted for 95.6 % of the total removal. H 2 O 2 is initially activated at the Co-N 5 site, which generates the active intermediate Co-OH groups. This Co-OH group then further activates H 2 O 2 , leading to the production of •O 2 - /•OOH. The newly produced •O 2 - /•OOH are instantaneously captured by neighboring Co-OH groups and subsequently converted into 1 O 2 . These adjacent catalytic sites could effectively capture and stabilize the short-lived radicals through the distance effect. and the intermediate Co-OH group in the reaction significantly reduces the energy barrier for H 2 O 2 conversion to •O 2 - /•OOH and 1 O 2 conversion by 0.26 eV and 11.12 eV, respectively. The efficiency of tetracycline degradation at 96 % even with the Cl - concentration as high as 7000 mg/L.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 8
·e202303088
·
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
·
催化
·
水处理
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Fan Wu,Xueyu Nie,Yulun Nie,Chu Dai,Xike Tian
As reported, PMS can be activated and decomposed into different reactive oxygen species such as 1 O 2 , • OH and SO 4 •- , besides, coupling of non-radical (PMS direct oxidation) and radical (SO 4 •- ) process could enhance the utilization efficiency of PMS. In this study, we proposed another strategy of 1 O 2 -based non-radical and • OH-based radical process using layered double hydrotalcite (MgAl-LDH and MgAlCu-LDH) to regulate the degradation, transformation and even mineralization of sulfamethoxazole. Compared with PMS direct oxidation , SMX removal efficiency was increased from 41.8% to 71.7% by 1 O 2 . However, there was almost no real degradation or mineralization since the ionization intermediates including C 10 H 12 N 3 O 4 S and C 7 H 9 N 3 O 5 S accumulated with reaction time according to DFT and LC-MSMS analysis. In comparison, 100% of SMX degradation was obtained via coupling 1 O 2 and • OH-radical process, in which the mineralization efficiency reached to 24.8%. Importantly, the above-mentioned intermediates of SMX were not detected and their accumulation were also significantly inhibited. Moreover, SMX degradation behavior and kinetics could be manipulated via direct oxidation , 1 O 2 and then • OH step by step, which was beneficial to enhance the PMS utilization efficiency. Finally, based on the results of zeta potential of MgAlCu-LDH, effect of solution pH on SMX degradation, the interfacial PMS activation process was responsible to regulate non-radical and radical process.
研究领域:
环境科学
·
化学
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
研究领域:
环境化学
·
电化学
·
催化
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·Vol. 23
·期 1
·1-23
·
IF 12.6
Zou Lan,Wang Rujing,Zhao Mengnan,Li Yuke,Sun Chen,Xie Jinjin,Chen Yan,Jing Qian,Mi Dandan,Shi Sanjun
Pyroptosis, a recently identified cellular demise regulated by gasdermin family proteins, is emerging as a promising avenue in cancer immunotherapy. However, the realm of light-controlled pyroptosis in cancer cells remains largely unexplored. In this study, we took a deliberate approach devoid of any chemical alterations to develop a novel photosensitizer called “pharmaceutical-dots (pharm-dots)” by combining nonemissive polymers (Poly (lactic-co-glycolic acid), PLGA) with nonfluorescent invisible molecules like curcumin, berberine, oridonin into PLGA nanoparticles (PLGA-NPs). Initially, our research commenced with a comprehensive mechanistic comparison study, consolidating fragmented information on optical mechanisms. This exploration revealed that surface passivation atoms play a dominant role in governing the fluorescence emission of PLGA-NPs. Remarkably, these new luminophores, composed of two non-inherently luminous components, exhibit a remarkable synergistic boost in photoluminescence through a “0 + 0 > 2” phenomenon. In-depth investigations uncovered that these luminous PLGA-NPs, capable of generating 1 O 2 , induce pyroptosis under photoexcitation conditions through the caspase-3/gasdermin E (GSDME) pathway. Simultaneously, our findings highlight PLGA-NPs as a novel optical formulation suitable for imaging, displaying substantial biological activity when paired with photoirradiation. This discovery holds the potential to facilitate the application of light-controlled pyroptosis in antitumor therapy, marking a promising stride toward innovative approaches in cancer treatment. Graphical abstract
研究领域:
癌症研究
·
生物光子学
·
纳米技术
·
免疫疗法
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuan Zhang,Kangping Cui,Xueyan Liu,Minshu Cui,Xing Chen,Yuchao Tang,Haiyang Li
Metal-based catalyst could be used for efficient peroxymonosulfate (PMS) activation, but inevitably suffered from metal ion leaching. Metal-free graphitic carbon nitride (g-C 3 N 4 ) materials that can activate PMS are more conducive for practical water treatment. In this study, g-C 3 N 4 with both N-defects and P-doping (CN-NP) was synthesized, which mainly produce singlet oxygen ( 1 O 2 ), and 97 % of 4-CP (4-Chlorophenol) was removed by CN-NP/PMS/Vis reaction system within 60 min. The active species was identified by quenching experiments and electron spin resonance (ESR) tests, and the origin of mainly active species was further verified by the concentration change of PMS during the reaction. It was verified by experiments and theoretical calculations that the introduction of N-defects led to the separation of photoinduced electron-hole pairs and improved photocatalytic activity. Notably, density functional theory (DFT) revealed that both N-defects and P-doping are electron-deficient sites, and P-doping acts as the main PMS adsorption site to promote the loss of electrons from PMS to generate 1 O 2 . In addition, the catalysts developed in this research were anticipated to be applied in real wastewater treatment, contributing to further comprehend the mechanisms of element doping and defect modification in g-C 3 N 4 activating PMS, and providing new insights for the design of PMS-activating catalysts.
研究领域:
环境科学
·
材料科学
·
催化
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yuantian Zhao,Zhiwei Zhou,Haikuan Yu,Xing Li,Jiawei Ren,Junyan Chen,Fei Qi
Developing carbonaceous composites with strong non-radical activity and recyclability is key for sustainable wastewater purification. Herein, a novel photocatalytic process was designed using zinc ferrite loaded on oxalic acid-modified powdered activated carbon (ZFO/OA/PAC) to activate persulfate (PDS) under visible light (VL) irradiation. ZFO was in-situ grown onto OA/PAC via C=O bridging, forming stable Zn/Fe–O–C bonds that suppressed magnetic agglomeration and enabled directional electron transfer. The optimized interfacial binding energy of 22.45 kcal/mol reduced the activation energy barrier, enhancing active site utilization and reaction kinetics through efficient electron cycling. With a narrow bandgap of 1.54 eV, 0.1 g/L ZFO/OA/PAC and 0.1 g/L PDS achieved 94.3% tetracycline (TC) removal under VL, with a kinetic constant 23.75 times higher than pristine ZFO. The process predominantly generated h + and 1 O 2 , the latter arising from superoxide conversion, PDS-induced functional group transformation, and oxygen-vacancy-mediated electron transfer. Photocatalysis also promoted Fe(III)/Fe(II) cycling, further aiding reactive oxygen species (ROS) formation. Seventeen intermediates were identified, with degradation and detoxification proceeding mainly through ring-opening, substitution, and ROS-driven molecular reconstruction. The magnetic ZFO/OA/PAC exhibits broad organic pollutants’ removal capability and effective adaptability to real water matrices. This work provides a paradigm for designing magnetic carbonaceous photocatalysts to leverage non-radical pathways, advancing scalable wastewater purification technologies.
研究领域:
环境科学
·
材料科学
·
化学工程
·
光催化
·
水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yilan Jiang,Peifang Wang,Tingyue Chen,Keyi Gao,Yiran Xiong,Yin Lu,Dionysios D. Dionysiou,Dawei Wang
Iron-based materials are difficult to produce single oxygen ( 1 O 2 ) efficiently from H 2 O 2 . Herein, we demonstrate that 1 O 2 production from H 2 O 2 can be manipulated by regulating the lattice distortion degrees of spinel ferrite through controlling the contents of Co and Ni in Co 1−x Ni x Fe 2 O 4 . Typically, NiFe 2 O 4 , which owns the lowest lattice distortion degree, can produce 1 O 2 as the dominated reactive oxygen species with·O 2 - as the intermediate. Due to the production of 1 O 2 , the NiFe 2 O 4 /H 2 O 2 system removes bisphenol A (BPA) completely within 180 min but removes only ∼ 4% of benzoic acid . In addition, the system demonstrates significant resistance to water matrix interference, as 50 mM of Cl - , NO 3 - , H 2 PO 4 - , and humic acid inhibited the BPA degradation by only ∼0%, ∼2%, ∼40%, and ∼3%, respectively. Our work may shed light for regulating the formation of 1 O 2 from H 2 O 2 through the rational design of iron-based catalysts for Fenton-like reactions.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Lulu Long,Changwei Bai,Xinyu Zhou,Shirong Zhang,Yanzong Zhang,Chao Chen,Jingsong He,Chun Song,Gang Yang
This study proposed a novel strategy to improve the activation efficiency of PMS by enhancing the utilization of side reactions. Electrocatalysis and PMS activation were coupled in the anode chamber. The electrons were extracted from the catalyst through the electroanode, and the excess low valence elements in the system were converted into high valence elements. Without restricting the activation of PMS, the activation efficiency of PMS was more effectively and comprehensively improved by enhancing the utilization of side reactions. An efficient electrocatalytic anode/Mn 2 O 3 /rGO/peroxymonosulfate (ECA/Mn 2 O 3 /rGO/PMS) system was established with Mn 2 O 3 /rGO as the anode. In this system, the anode current improved the catalyst utilization, which directly converts the excess rGO-C = O, Mn(II) and Mn(III) into rGO-C + -O, Mn(III) and Mn(IV), thereby increasing the yields of •OH, SO 4 • - , and 1 O 2 during PMS activation. Overall, this study provides a novel strategy for improving the activation efficiency of PMS, and has great potential to be widely applied in actual environment remediation.
研究领域:
环境科学
·
化学工程
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yong Chen,Huiping Zeng,Jiaxin Xu,Dong Li,Jie Zhang
Currently, there are well-operated iron removal water plants in the northeast region of China. Among them, the backwash process produces a large amount of iron-containing sludge (IS) year by year, which can cause some harm to the environment if not treated. The main form of existence for IS is amorphous γ-FeOOH, and this work demonstrates that IS is a natural and highly active catalyst for periodate(PI). Moreover, IS showed strong stability in environmental factor effects and reproducibility experiments. EPR with quenching experiments proved that IS could activate PI to produce •OH, O 2 •− , 1 O 2 , and IO 3 • . In the degradation experiments where methylene blue was chosen as the model pollutant, IO 3 • , and 1 O 2 were the substances that served the prominent role in degradation. This work provides an inexpensive and feasible way to dispose of waste iron-containing sludge from water plants and provides fundamental insights into the degradation mechanism of organic pollutants through the activation of PI by IS.
研究领域:
环境科学
·
化学工程
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Hong Yechun,Yu Zongjun,Zhou Qian,Chen Chunyu,Hao Yuqiong,Wang Zhen,Zhu Jian-Kang,Guo Hongwei,Huang Ancheng C.
Nicotinamide adenine dinucleotide (NAD + ) is a redox cofactor and signal central to cell metabolisms. Disrupting NAD homeostasis in plant alters growth and stress resistance, yet the underlying mechanisms remain largely unknown. Here, by combining genetics with multi-omics, we discover that NAD + deficiency in qs-2 caused by mutation in NAD + biosynthesis gene- Quinolinate Synthase retards growth but induces biosynthesis of defense compounds, notably aliphatic glucosinolates that confer insect resistance. The elevated defense in qs-2 is resulted from activated jasmonate biosynthesis, critically hydroperoxidation of α-linolenic acid by the 13-lipoxygenase (namely LOX2), which is escalated via the burst of chloroplastic ROS-singlet oxygen ( 1 O 2 ). The NAD + deficiency-mediated JA induction and defense priming sequence in plants is recapitulated upon insect infestation, suggesting such defense mechanism operates in plant stress response. Hence, NAD homeostasis is a pivotal metabolic checkpoint that may be manipulated to navigate plant growth and defense metabolism for stress acclimation.
研究领域:
植物学
·
遗传学
·
代谢组学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Wenting Wu,Congcong Han,Qinhua Zhang,Qinggang Zhang,Zhongtao Li,David J. Gosztola,Gary P. Wiederrecht,Mingbo Wu
Carbon nitride as a metal-free conjugated polymer exhibits an intriguing prospect for the design of advanced photosensitizers for singlet oxygen ( 1 O 2 ) generation. However, the intersystem crossing (ISC) process is quite insufficient in carbon nitride, limiting the 1 O 2 generation. Here, we report a facile and general strategy to confined benzophenone as a heavy atom-free spin converter dopant in carbon nitride via the facile copolymerization . With proper energy level matching between the heavy atom-free spin converter and various ligands based on carbon nitride precursors, the proper combination can decrease the singlet-triplet energy gap (ΔE ST ) and hence generate 1 O 2 effectively. Due to its significant and selectivity for 1 O 2 generation, the as-prepared carbon nitride-based photosensitizer shows a high selective photooxidation activity for 1,5-dihydroxy-naphthalene (1,5-DHN). The product yield reached 71.8% after irradiation for 60 min, which was higher than that of cyclometalated Pt II complexes (53.6%) in homogeneous photooxidation. This study can broaden the application of carbon nitride in the field of selective heterogeneous photooxidation due to simple operation, low cost, and high efficiency, making it a strong candidate for future industrialization.
研究领域:
材料科学
·
光化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）