APPLIED COMPOSITE MATERIALS
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2021
·Vol. 29
·期 2
·729-743
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IF 2.181
Huo Yanqiu,Ge Huan,Lin Changhong,Ying Puyou,Huang Min,Zhang Ping,Yang Tao,Liu Gang,Wu Jianbo,Levchenko Vladimir
The development of polymer-based composites with self-healing and recyclable capability has attracted the attention of several researchers for resource recycling and environment protection. In this work, Halloysite nanotubes (HNTs) reinforced polyurethane materials (PU) with self-healing and recyclable ability were constructed by in situ polymerization method. The mechanical, thermal amd morphological properties of PU and related composites were studied. The morphology of samples fracture surface ensured the homogeneous dispersion of HNTs in the polymer matrix. Moreover, thermal stability was improved with the incorporation of the HNTs. The tensile test showed strength increased with HNTs content increased. The tensile strength of composites increases from 23.38 to 34.92 MPa at 2 wt% HNTs. Therefore, the designed strategy provides a simple approach for preparing high mechanical properties, reprocessing and self-healing ability polyurethane composites.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Wenjie Wu,Liang Bai,Yenan Song,Yuanting Su,Kai Jiang,Haitao Sun,Guangyin Zhen,Yan Shen,Qinghong Yuan,Zhuo Sun
Graphene-based catalysts have been widely applied for catalytic ozonation. However, as it is difficult to obtain graphene with high structural precision, it is currently unfeasible to comprehend the relationships between the intrinsic structure of the layered carbon catalysts with its catalytic activities. Here, an advanced plasma-assisted etch strategy was used to fine tune the ozonation activity of monolayered graphene films by tailoring the defect types. Raman mapping indicated that the defects of the as-prepared monolayered graphene films were predominantly sp3, vacancy, and boundary-type defects, respectively. The roles and contributions of these active defects in manipulating the oxidative potential of monolayered graphene films were revealed by quenching experiments, electron paramagnetic resonance results, and density functional theory calculations. The catalytic results showed that the monolayered graphene films with boundary-like defects exhibited the best catalytic performance toward the degradation of sulfamethoxazole. This work contributes new insights into the design of high-efficiency carbonaceous catalysts by structuring additional defective sites.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yangke Long,Jian Dai,Shiyin Zhao,Shixin Huang,Zuotai Zhang
Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as Co@NC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation , surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation.
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APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Jinping Liang,Ling Fu
Persulfate-based advanced oxidation process (PS-AOP) is a promising technology for in-depth wastewater treatment. Here, Co 3 O 4 quantum dots (QDs) decorated hierarchical C@Co 3 O 4 (C@Co 3 O 4 -Q5) was prepared by a facile route. The crystalline structure, micrograph and chemical composition of C@Co 3 O 4 -Q5 were characterized by XRD, SEM, TEM and XPS. Taking Rhodamine B (RhB) as a model contaminant, the influences of process parameters on the degradation performance were evaluated. Detailed reaction kinetics investigation indicated that, at elevated temperatures higher than 30 °C, RhB degradation rate approximately follows this expression: r = 1.022 × 1 0 7 e x p ( - 47850 / R T ) [ R h B ] [ P M S ] 0.36 , whereas the real energies for catalytic activation ( Eac ) and heat activation ( Eah ) were 16.231 kJ·mol −1 and 31.62 kJ·mol −1 , respectively. Reactive oxygen species (ROS) quenching experiments and EPR tests suggested that not the general held radical SO 4 − but the downstream OH and the nonradical ROS 1 O 2 co-contribute to RhB mineralization. Meanwhile, PMS activation mechanisms referring to OH and 1 O 2 generation were elaborated based on XPS discussion. It was revealed that Co 3 O 4 quantum dots and oxygen functional groups and/or oxygen defects on carbon surface cooperate to generate ROS. Additionally, 5 successive cycles confirmed C@Co 3 O 4 -Q5′s high stability and reusability. These findings provided new insights into carbon-loaded QDs catalysts for PMS-mediated micropollutants removal.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Jiayi Li,Zhaokun Xiong,Yahan Yu,Xinhao Wang,Hongyu Zhou,Bingkun Huang,Zelin Wu,Chunxiu Yu,Tingting Chen,Zhicheng Pan,Gang Yao,Bo Lai
In this study, the removal efficiency of carbamazepine (CBZ) was significantly improved in an electro-Fenton system without any extra oxidant (e.g., O 2 or H 2 O 2 ) in the presence of sodium molybdate (EF-Na 2 MoO 4 system). The slow release of iron ions of EF-Na 2 MoO 4 system greatly reduced the generation of iron sludge and effectively promoted the utilization of iron ions. The pseudo-first-order rate constants ( k obs ) for CBZ removal by EF-Na 2 MoO 4 process (0.0417 min −1 ) was much higher than those of sole electrolysis (0.0007 min −1 ) and EF-Na 2 SO 4 systems (0.0044 min −1 ). Meanwhile, the total iron concentration in EF-Na 2 MoO 4 process was 4.93 mg/L for 60 min, which was extremely lower than that of EF-Na 2 SO 4 process (271.22 mg/L). Besides, the primary reactive species was proposed to be superoxide radical (O 2 − ), while hydroxyl radical ( OH) and MoO 2 (O 2 ) 2 2− acted as the secondary reactive species. Our work elucidated the possible mechanism that the slow release of iron ions promotes pollutants degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Wentao Zhang,Wenguang Huang,Jiyuan Jin,Yonghai Gan,Shujuan Zhang
The importance of singlet oxygen ( 1 O 2 ) in synthesis of fine chemicals, inactivation of viruses and bacteria, degradation of pollutants, and photodynamic therapy has promoted the research on photocatalytic generation of 1 O 2 . Metal-organic frameworks (MOFs), owing to the tunable structure, are good candidate photocatalysts for 1 O 2 generation. However, due to the poor visible-light absorption capacity and the invalid recombination of charge carriers, the 1 O 2 generation yields of most MOFs are still limited. Here, we demonstrate that β -diketone anchoring could improve the photocatalytic generation of 1 O 2 by MIL-125 through enhanced energy transfer. The enhanced energy transfer was attributed to both the narrowed bandgap and the diketone-derived oxygen vacancies, which function as the trapping sites for charge carriers. The results here shed light on the generation of 1 O 2 by visible-light-responsive MOFs and provide a new strategy for the design of MOFs-based photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Chang-Long Tan,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Highly efficient photodriven conversion from biomass-derived platform chemicals to value-added chemical feedstocks and clean fuel hydrogen (H 2 ) possesses immense potential to cope with the existing energy and environmental problems. We herein report a facile approach combining hydrothermal method and photodeposition method for fabricating diverse sulfide-based cocatalysts (MoS 2 , NiS and WS 2 ) decorated ZnIn 2 S 4 (ZIS) for simultaneous exploitation of photogenerated electrons and holes, effectively achieving the oxidation of furfuryl alcohol (FOL) cooperative with H 2 evolution in one photoredox cycle. The results show the optimal binary MoS 2 -ZIS composites can obtain almost 7 times yield of products (furfural and H 2 ) as high as that of blank ZIS. Notably, compared with previous reports in literatures, our present MoS 2 -ZIS shows the best performance in this photoredox dual reaction. As a relay station for electrons, cocatalysts facilitate the separation and transfer of photogenerated charge carriers in the composites, therefore prominently improving the photocatalytic performance. We anticipate that the present work can offer insights to guide the design of photoredox reaction systems for efficient valorization of biomass-derived platform chemicals.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
·
IF 9.028
Wei Wu,Shishu Zhu,Xiaochen Huang,Wei Wei,Chao Jin,Bing-Jie Ni
Persulfate (PS) activation on biochar (BC) is a promising technology for degrading the aqueous organic contaminants. However, the complexity of activation mechanisms and components in biomass that used to produce BC makes it difficult to predict the performance of PS activation. In this study, we employed eight sludges as the representative biomass that contained absolutely different organic or inorganic components. Results showed that the elemental composition, surface properties, and structures of the sludge-derived BCs (SBCs) clearly depended on the inherent components in the sludges. The intensities of persistent free radicals (PFRs) in the electron paramagnetic resonance (EPR) correlated positively with N-containing content of sludges as electron shuttle, but negatively with the metal content as electron acceptor. Linking with PFRs as crucial sites of triggering a radical reaction, a poly-parameter relationship of predicting PS activation for organic degradation using the sludge components was established (kobs,PN = 0.004 × Cprotein + 0.16 × CM–0.895 −0.118). However, for the PS activation on those SBCs without PFRs, this redox process only relied on the sorption or conductivity-related characteristics, not correlating with the content of intrinsic components in biomass but with pyrolysis temperatures. This study provided insightful information of predicting the remediation efficiency of PS activation on BCs and further understanding the fate of contaminants and stoichiometric efficiency of oxidants in a field application.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Yi Wang,Qingjie Ji,Jixiang Xu,Jun Wan,Lei Wang
In this study, N-doped porous carbon materials embedded with NiN x species (Ni@NC) were fabricated via the pyrolysis of Ni-doped zeolitic imidazolate frameworks-8 (ZIF-8) at the temperature of 900 °C. The obtained Ni@NC-1 catalyst exhibited excellent activity in activating the peroxydisulfate (PDS) that was used for removing tetracycline (TC). The catalytic system exhibited good stability, wide pH adaptation, and high resistance to the operational environment. It was supposed that NiN x species could attach to PDS and act as electron acceptors to receive the electrons for activating the PDS, thus generating highly reactive superoxide radicals (⋅O 2 − ) and singlet oxygen ( 1 O 2 ) species for rapid degradation of TC. The electron transfer and dissolved oxygen-derived ⋅O 2 − were also responsible for the degradation of TC. In addition, the Ni@NC-1/PDS system exhibited high efficiency for removing oxytetracycline, ciprofloxacin, or levofloxacin. The results of this study would promote the design of other MOFs-derived carbon-encapsulated metal species for efficiently activating persulfate to remove antibiotics from the wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jianan Yu,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin
Fenton-like catalysis has received much attention as the promising technology for organic pollutant degradation, whereas it suffers from low atomic utilization, poor catalysts durability and difficult after-treatment to hamper the catalytic oxidation activity. Herein, a Fe– and nitrogen-codoped carbon (Fe–N–C) originated from nanocellulose-based hydrochar, nitrogen source, and iron salt precursor was developed for improved PMS activation and identification of exclusive role of each species. The catalyst formed with interconnected bamboo-shaped 3D tubular structures and high Fe-doping level (up to ~9.0 wt%) not only realized excellent efficiencies in oxidative degradation of various aromatic pollutants, but was also endowed with high durability and stability toward PMS activation. Compared with that of the control catalysts only comprising either C–N network or supported Fe nanoparticles (Fe–C) with Fe IV –oxo complex sites, the co-existent active sites of Fe–N configuration and atomic Fe cluster in Fe–N–C could simultaneously improve the graphitization degree, and act as a “support” for constructing the stable structure. It is likely that the coordinated Fe–N formed with annealing process is devoted to decompose PMS by radical generation for pollutants degradation via a radical oxidation process; while the enhanced C–N bonded with graphitic N contribute to produce 1 O 2 through the nonradical processes interacted with PMS. This Fe–N–C/PMS-coupled process provided a designed strategy to construct the highly active and stable metal-nitrogen-codoped hydrothermal carbons, and deepened insights on structure-activity-stability relationship for persulfate-based environmental remediation.
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Bioactive Materials
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2021
·
IF 14.593
Jie Yu,Sha Liu,Yupeng Wang,Xidong He,Qingfei Zhang,Yanxin Qi,Dongfang Zhou,Zhigang Xie,Xiaoyuan Li,Yubin Huang
The combination of tumor ablation and immunotherapy is a promising strategy against tumor relapse and metastasis. Photothermal therapy (PTT) triggers the release of tumor-specific antigens and damage associated molecular patterns (DAMPs) in-situ. However, the immunosuppressive tumor microenvironment restrains the activity of the effector immune cells. Therefore, systematic immunomodulation is critical to stimulate the tumor microenvironment and augment the anti-tumor therapeutic effect. To this end, polyethylene glycol (PEG)-stabilized platinum (Pt) nanoparticles (Pt NPs) conjugated with a PD-L1 inhibitor (BMS-1) through a thermo-sensitive linkage were constructed. Upon near-infrared (NIR) exposure, BMS-1 was released and maleimide (Mal) was exposed on the surface of Pt NPs, which captured the antigens released from the ablated tumor cells, resulting in the enhanced antigen internalization and presentation. In addition, the Pt NPs acted as immune adjuvants by stimulating dendritic cells (DCs) maturation. Furthermore, BMS-1 relieved T cell exhaustion and induced the infiltration of effector T cells into the tumor tissues. Thus, Pt NPs can ablate tumors through PTT, and augment the anti-tumor immune response through enhanced antigen presentation and T cells infiltration, thereby preventing tumor relapse and metastasis.
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ChemCatChem
·
2021
·Vol. 13
·期 19
·4164-4181
·
IF 5.686
Qiuli Fu,Shibo Yang,Ping Ning,Rongrong Miao,Liang He,Qingqing Guan
Graphical Selective hydrogenation : In rubber seed shell porous biochar supported Cu−Ni bimetals, the formed Cu 1 Ni 3 alloy stabilized the excessive Cu species which were in the lattice on the inner/outer surfaces of the rss AC support. The catalytic activity is retained, ensuring that the catalyst would neither be oxidized nor aggregated severely. The prepared high-efficiency Cu 1 Ni 1 / rss AC catalyst catalyzed the hydrogenation reaction of FAL to produce FOL, THFA and 2-MF. Using cheap Cu-based catalysts for highly selective hydrogenation of furfural (FAL) is of great importance of upgrading this biomass-derived platform molecule but is still challenging for large-scale application due to the low conversion efficiency and the easy aggregation of Cu active sites. To address these issues, a nitrogen-autodoped porous biochar derived from rubber seed shell ( rss AC) was fabricated for anchoring Cu sites on a nanoscale. Moreover, by the co-crystallization strategy of Cu and the second metal (M, M=Ni, Zn, Co, Ce), stable Cu−M nanoalloys were constructed on the surface of the rss AC support. The FAL hydrogenation experiments showed that the type, proportion and loading amount of the second metal had great effect on the catalytic efficiency. Compared with the other metals, Ni-doped Cu/ rss AC catalyst exhibited the best hydrogenation performance due to their extraordinary adsorption and activation capacity for hydrogen. Further, the highest catalytic efficiency was observed using 20 % Cu 1 Ni 1 /rss AC catalyst. The characterization results showed that the key to its success was highly-dispersive anchoring of the CuNi active sites onto the inner/outer surface of the nanopores of rss AC support by the strong interaction between the surface N-containing functional groups and metals. Of note, the formed CuNi alloys with the Cu/Ni atomic ratio of 1 : 3 played an important role in the stabilization of the adjacent nano-dot matrix Cu 0 species. Kinetic test indicated that the formation step of furfuryl alcohol (FOL) from FAL was still the key step and the hydrogenation products can be converted between FOL and tetrahydrofurfuryl alcohol (THFA). The life evaluation test showed that the catalyst still kept high activity and selectivity after being reused five times. The advanced synthesis method co-using N-doped support anchoring and the second metal alloying strategy sheds light on preparing effective catalysts for hydrogenation of biomass-based compounds.
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