JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yu Liu,Linlin Qin,Yiming Qin,Tong Yang,Haoran Lu,Yulong Liu,Qiqi Zhang,Wenyan Liang
Nitrogen-containing heterocyclic compounds (NHCs) are hazardous, toxic, and persistent pollutants, thereby requiring urgent solutions. Herein, ZIF-67 was compounded with powder-activated carbon (PAC) to prepare Co/NC/PAC (NC i.e. nitrogen-doped carbon) particle electrodes for the electrocatalytic treatment of pyridine and diazines . Co/NC/PAC reflected the confinement of Co 3 O 4 /CoN/Co 0 into the N-doped graphitic-carbon layer to generate both pyrrolic-N and graphitic-N active sites. Under the optimal conditions (0.3 A, 12 mL min −1 , and initial pH 7.00), the degradation of four NHCs realized 90.2–93.7% efficiencies. The number and position of N atoms in NHCs directly affected the degradation efficiency. The following increasing order of facilitated degradation was recorded: pyridazine < pyrimidine < pyrazine < pyridine. The as-obtained Co/NC/PAC possessed the direct redox effect on NHCs, achieving fast electrocatalytic rate. Species like ·OH and H* were detected in Co/NC/PAC system with contributions to NHCs degradation estimated to 24% and 34%, respectively. Density functional theory (DFT) calculations revealed H* susceptible to attacking the N position, while the meta-position of C was subject to hydroxyl radical (·OH) addition. Overall, degradation of NHCs was achieved by hydro-reduction, oxidation , ring opening cleavage, hydroxylation, and mineralization. Ring-cleavage and mineralization of NHCs provided a novel electrochemical strategy to refractory wastewater treatment .
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
·
IF 8.7
Ziwei Guo,Huan He,Kunqian Liu,Shicheng Yang,Zihui Li,Chaochao Lai,Zhicheng Liao,Xiaomin Ren,Bin Huang,Xuejun Pan
Insights into COVID-19 antivirals’ environmental fate and ecological risk are urgently required due to their increasing concentrations in aquatic environments, which have rarely been studied. Herein, we first investigated the photochemical transformation and the resulting alterations in toxicity of arbidol, an antiviral drug with relatively higher toxicity. The photolysis of arbidol was rapid with a rate constant of 0.106 min −1 due to its superior ultraviolet light absorption , in which the direct photolysis was predominated with a contribution of 91.5%. Despite its substantial photolysis, only 14.45% of arbidol was mineralized after 100 min, implying that arbidol and its products might have a long-term impact on aquatic environment. It was inferred that arbidol was photolyzed mainly via the loss of thiophenol, bromine, and alkylamine, based on twelve photolytic products identified. Notably, the experimental results demonstrated that the photolysis process increased the acute toxicity of arbidol, and the toxicity prediction indicated that the ecotoxicity of two photolytic products was very high with LC 50 values below 0.1 mg/L. Due to the co-effect of multiple constituents, the photolytic rate observed in wastewater treatment plant effluent and in river water was comparable to that in ultra-pure water, while it was slightly enhanced in lake water. The presence of dissolved organic matter suppressed arbidol photolysis, while NO 3 − exhibited a promotion effect. These results would be of great significance to assess the fate and risk of COVID-19 antivirals in natural aquatic environments.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Weiting Yu,Dezheng Yang,Rendan Zhu,Luzhen Liu,Yan Yu,Juntao Tang,Zhiqiao He,Jiexu Ye,Shuang Song
The photoassisted electrochemical CO2 reduction reaction (CO2RR) toward CO is considered one of the most promising routes of CO2 utilization. In this work, 2,6-diaminopyridine (2,6-DAP) with both the pyridine ring and the –NH2 functional group is utilized for the first time to functionalize the surface of the electrode. The p-Si/Ag/2,6-DAP electrode has been identified as a good catalyst with relatively high activity and CO selectivity at a low overpotential as well as good stability. The Faradaic efficiency of CO is 84.56% at an optimized potential of −0.9 V vs reversible hydrogen electrode (RHE). A synergistic mechanism has been proposed for the enhanced catalytic performance of p-Si/Ag/2,6-DAP in the CO2RR. Ag facilitates the reduction of CO2 to produce CO. 2,6-DAP helps CO2 adsorption and inhibits the competitive hydrogen evolution reaction accompanying the CO2RR under low potentials.
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FUEL
·
2023
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IF 7.4
Meiyu Liu,Xinyu Sun,Yiming Zhang,Ye Yang,Yucai Qin,Binbin He,Yi Mei,Yun Zu
Propane dehydrogenation (PDH) is one of the most effective methods for intentional (“on-purpose”) propylene production. Isolated Sn sites on open supports exhibit considerable PDH performance comparable to that of industrial Pt- and Cr-based catalysts, but the loss of Sn is inevitable. Herein, highly dispersed and stable NiSn subnanoclusters encapsulated within the channels of silicalite-1 zeolite are fabricated through a one-step hydrothermal synthesis in this work. The as-prepared Ni 1 Sn 1 @S-1 zeolite catalyst exhibits outstanding PDH performance with considerable propylene formation rate (ca. 12.3 mmol∙g cat -1 ∙h −1 ) and high propylene selectivity (>88 %). Most significantly, no Sn loss is detected after three regeneration cycles. Structural elucidation of NiSn sites on catalysts, by HRTEM, H 2 -TPR, FTIR and XPS characterizations confirms that the Ni sites embedded in the geminal silanols of zeolitic framework play a vital role in anchoring Sn species and preventing the active sites from losing and sintering. The cooperative action of robust NiSn subnanoclusters is conducive to the selective C–H activation and the propylene desorption. A plausible dehydrogenation mechanism is revealed by in situ infrared spectroscopy. This study on siliceous zeolite confined NiSn catalysts delivers an insight into the nature of selective and stable NiSn sites involved in the PDH reaction.
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STRUCTURE
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2023
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IF 5.7
Jin Dong,Han Xiao,Jia-Nan Chen,Bai-Feng Zheng,Yu-Ling Xu,Meng-Xi Chen,Wen-Chao Yang,Hong-Yan Lin,Guang-Fu Yang
4-Hydroxyphenylpyruvate dioxygenase (HPPD) has attracted increasing attention as a target for treating type I tyrosinemia and other diseases with defects in tyrosine catabolism. Only one commercial drug, 2-(2-nitro-4-trifluoromethylbenzoyl)-1, 3-cyclohexanedione (NTBC), clinically treat type I tyrosinemia, but show some severe side effects in clinical application. Here, we determined the structure of human HPPD-NTBC complex, and developed new pyrazole-benzothiadiazole 2,2-dioxide hybrids from the binding of NTBC. These compounds showed improved inhibition against human HPPD, among which compound a10 was the most active candidate. The Absorption Distribution Metabolism Excretion Toxicity (ADMET) predicted properties suggested that a10 had good druggability, and was with lower toxicity than NTBC. The structure comparison between inhibitor-bound and ligand-free form human HPPD showed a large conformational change of the C-terminal helix. Furthermore, the loop 1 and α7 helix were found adopting different conformations to assist the gating of the cavity, which explains the gating mechanism of human HPPD.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2023
·Vol. 24
·期 19
·14805
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IF 5.6
Xiao Xia,Jun Ma,Fei Liu,Haifeng Cong,Xingang Li
In the heavy petroleum industry, the development of efficient demulsifiers for the effective breaking of interfacially active asphaltenes (IAA)-stabilized water-in-heavy oil (W/HO) emulsions is a highly attractive but challenging goal. Herein, a novel nitrogen and oxygen containing demulsifier (JXGZ) with strong hydrogen bonding has been successfully synthesized through combining esterification, polymerization and amidation. Bottle tests indicated that JXGZ is effectual in quickly demulsifying the IAA-stabilized W/HO emulsions; complete dehydration (100%) to the emulsions could be achieved in 4 min at 55 °C using 400 ppm of JXGZ. In addition, the effects of demulsifier concentration, temperature and time on the demulsification performance of JXGZ are systematically analyzed. Demulsification mechanisms reveal that the excellent demulsification performance of JXGZ is attributed to the strong hydrogen bonding between JXGZ and water molecules (dual swords synergistic effect under hydrogen bond reconstruction). The interaction of the “dual swords synergistic effect” generated by two types of hydrogen bonds can quickly break the non-covalent interaction force (π-π stacking, Van der Waals force, hydrogen bonds) of IAA at the heavy oil–water interface, quickly promote the aggregation and coalescence of water molecules and finally achieve the demulsification of W/HO emulsions. These findings indicate that the JXGZ demulsifier shows engineering application prospects in the demulsification of heavy oil–water emulsions, and this work provides the key information for developing more efficient chemical demulsifiers suitable for large-scale industrial applications.Keywords:demulsifier;hydrogen bonds;interactions;water-in-heavy oil emulsions
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Acta Biomaterialia
·
2023
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IF 9.7
Yifei Wang,Jia Wang,Yunke Jiao,Kangli Chen,Tianhao Chen,Xinping Wu,Xingwu Jiang,Wenbo Bu,Changsheng Liu,Xue Qu
Chemodynamic therapy (CDT) based on generating reactive oxygen species (ROS) is promising for cancer treatment. However, the intrinsic H 2 O 2 is deficient for CDT, and glutathione (GSH) eliminates ROS to protect tumor cells from ROS cytotoxicity. Herein, we propose a strategy to switch the electron flow direction of GSH for O 2 reduction and ROS generation rather than ROS clearance by using P(DA-Fc) nanoparticles , which are polymerized from ferrocenecarboxylic acid (Fc) coupled dopamine. P(DA-Fc) NPs with phenol-quinone conversion ability mimic NOX enzyme to deprive electrons from GSH to reduce O 2 for H 2 O 2 generation; the following •OH release can be triggered by Fc. Semiquinone radicals in P(DA-Fc) are significantly enhanced after GSH treatment, further demonstrated with strong single-electron reduction ability by calculation. In vitro and in vivo experiments indicate that P(DA-Fc) can consume intrinsic GSH to produce endogenous ROS; ROS generation strongly depends on GSH/pH level and eventually causes tumor cell death. Our work makes the first attempt to reverse the function of GSH from ROS scavenger to ROS producer, explores new roles of PDA-based nanomaterials in CDT beyond photothermal reagents and drug carriers, and provides a new strategy to improve the efficiency of CDT. Statement of Significance P(DA-Fc) nanoparticles performing tumor microenvironment response capacity and tumor reductive power utilize ability were fabricated for CDT tumor suppression. After endocytosis by tumor cells, P(DA-Fc) deprived GSH of electrons for H 2 O 2 and •OH release, mimicking the intrinsic ROS production conducted by NADPH, further inducing tumor cell necrosis and apoptosis. Our work makes the first attempt to reverse the function of GSH from ROS scavenger to producer, explores new functions of PDA-based nanomaterials in CDT beyond photothermal reagents and drug carriers, and provides a new strategy to improve CDT efficiency.
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Journal of Cleaner Production
·
2023
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IF 11.1
Shiwei Chen,Yonghao Hu,Dongfang Gao,Chaofeng Zhu,Bing Li,Zhenhua Wang,Xinjing Pan
Aiming to realize sustainable development and reduce environmental pollution , scientists have been on searching for bio-based materials derived from renewable resources to replace petroleum-based materials. Herein, a bio-based polyimide aerogel derived from 2,5-furandicarboxylic acid was synthesized successfully via supercritical fluid drying. The bio-based polyimide aerogel had mesoporous structure and a large specific surface area (220 m 2 /g), which were highly advantageous to adsorption and photocatalysis . The bio-based polyimide aerogel possessed fast adsorption behavior (within 1 s), outstanding durability (200 cycles of adsorption and desorption), and a self-cleaning property. The bio-based polyimide aerogel could also realize continuous and rapid separation of organic solvent and water with the aid of a vacuum pump. Importantly, the bio-based polyimide aerogel exhibited superelastic (rapid recovery after 90% strain) and anti-fatigue performance (compressive strength remained 96% after 100 cycles). Moreover, the bio-based polyimide aerogel displayed effective photocatalytic activity under visible light. The possible degradation mechanism was also proposed, and radical quenching tests demonstrated that the generation of h + and ·O 2 − was the key to photocatalytic degradation . Considering its environmental friendliness and excellent properties, bio-based polyimide aerogel provides a promising solution for oil/water separation and photocatalysis.
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Frontiers of Optoelectronics
·
2023
·Vol. 16
·期 1
·1-10
·
IF 5.4
Zhao Xinzhao,Li Mingyu,Ma Tianjun,Yan Jun,Khalaf Gomaa Mohamed Gomaa,Chen Chao,Hsu Hsien-Yi,Song Haisheng,Tang Jiang
Infrared solar cells are more effective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region, thus also at broadening the absorption spectra and improving power conversion efficiency. PbS colloidal quantum dots (QDs) with tunable bandgap are ideal infrared photovoltaic materials. However, QD solar cell production suffers from small-area-based spin-coating fabrication methods and unstable QD ink. Herein, the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory. We further studied a mixed solvent system using dimethylformamide and butylamine, compatible with the scalable manufacture of method-blade coating. Based on the ink system, 100 cm 2 of uniform and dense near-infrared PbS QDs (~ 0.96 eV) film was successfully prepared by blade coating. The average efficiencies of above absorber-based devices reached 11.14% under AM1.5G illumination, and the 800 nm-filtered efficiency achieved 4.28%. Both were the top values among blade coating method based devices. The newly developed ink showed excellent stability, and the device performance based on the ink stored for 7 h was similar to that of fresh ink. The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices. Graphical Abstract
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Nano Energy
·
2023
·
IF 17.6
Boyuan Hu,Jian Zhang,Yulin Yang,Yayu Dong,Jiaqi Wang,Wei Wang,Kaifeng Lin,Debin Xia,Ruiqing Fan
Under the stimulation of external factors, the ions with small activation energies could escape from the surface of perovskite , aggravating the defects at the interfaces and deteriorating the perovskite solar cells (PSCs). Here, we report a novel strategy utilizing a tailored organometallic molecule (bis-ferrocenyl-carboxylate-hexadecafluorodecyl, namely Fc-16 F) interlayer to functionalize the perovskite/hole transport layer interface , which simultaneously blocks the migration pathways of ions and facilitate the charge extraction at the interface. The electron-absorbing substituents (carboxyl groups and a long C-F chain) are introduced to strengthen the redox properties of ferrocene units, limit self-migration, and enhance hydrophobicity . With the strengthened oxidation driving force and the tight and dense hydrogen bond networks formed between Fc-16 F and organic cations, Fc-16 F could efficiently recover the Pb, I vacancies, inhibit the diffusion of defect-induced by-products (I 2 ), and stabilize the components on the surface. The champion device modified with Fc-16 F interlayer yields a remarkable power conversion efficiency (PCE) of 23.02% as well as superior humidity and long-term stabilities. The Fc-16 F-modified PSCs retain an outstanding 83.3% of its initial PCE over 1200 h under high humidity (60% RH) and retain over 90% of its initial PCE after aging in the N 2 atmosphere for over 2000 h.
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JACS Au
·
2023
·
IF 8
Chunyu Yuan,Hongfei Yin,Huijun Lv,Yujin Zhang,Jing Li,Dongdong Xiao,Xiaoyong Yang,Yongzheng Zhang,Ping Zhang
Given the rapid recombination of photogenerated charge carriers and photocorrosion, transition metal sulfide photocatalysts usually suffer from modest photocatalytic performance. Herein, S-vacancy-rich ZnIn2S4 (VS-ZIS) nanosheets are integrated on 3D bicontinuous nitrogen-doped nanoporous graphene (N-npG), forming 3D heterostructures with well-fitted geometric configuration (VS-ZIS/N-npG) for highly efficient photocatalytic hydrogen production. The VS-ZIS/N-npG presents ultrafast interfacial photogenerated electrons captured by the S vacancies in VS-ZIS and holes neutralization behaviors by the extra free electrons in N-npG during photocatalysis, which are demonstrated by in situ XPS, femtosecond transient absorption (fs-TA) spectroscopy, and transient-state surface photovoltage (TS-SPV) spectra. The simulated interfacial charge rearrangement behaviors from DFT calculations also verify the separation tendency of photogenerated charge carriers. Thus, the optimized VS-ZIS/N-npG 3D hierarchical heterojunction with 1.0 wt % N-npG exhibits a comparably high hydrogen generation rate of 4222.4 μmol g–1 h–1, which is 5.6-fold higher than the bare VS-ZIS and 12.7-fold higher than the ZIS without S vacancies. This work sheds light on the rational design of photogenerated carrier transfer paths to facilitate charge separation and provides further hints for the design of hierarchical heterostructure photocatalysts.
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Nanotechnology Reviews
·
2023
·Vol. 12
·期 1
·
IF 7.4
Wen-Juan Zhang,Ye-Zhi Ding,Ya-Xian Wang,You-Liang Wang,Yu-Long Fei,Meng-Yu Ran
The pollution of silver ion (Ag( i )) has become a serious environmental threat and hazard to ecosystem and human health. Thus, the nanoscale zero valent iron (nZVI)-doped polypyrrole-based carbon nanotube (nZVI/CNT) composites were synthesized by a facile method to remove Ag( i ) from wastewater due to the toxicity and scarcity nature of Ag( i ). In this process, Fe 3+ initiated the self-assembly of polypyrrole tubes in the presence of methyl orange, while it also served as an iron source generated nZVI/CNTs by carbothermal reduction method. The nZVI/CNT composites exhibited a homogeneous tubular structure, and the nZVI formed were uniformly dispersed in the nZVI/CNT composites. The nZVI/CNT composites were used as an adsorbent for the removal of Ag( i ) and showed a higher adsorption capacity compared to nZVI and CNTs, with a maximum adsorption capacity of 522.41 mg g −1 . Ag( i ) was adsorbed on nZVI/CNT composites by ion exchange and chelation, where Ag( i ) was reduced to non-toxic Ag due to the redox reaction among pyrrolic-N, nZVI, and Ag( i ). The adsorption process of Ag( i ) on nZVI/CNT composites was dominated by monolayer adsorption. According to our results, nZVI/CNT composites can be used as economical treatment for wastewater containing Ag( i ).
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