CHEMOSPHERE
·
2022
·
IF 8.943
Wei Li,Huanyu Yue,Chunyan Zhang,Junyu Hu,Qiaoli Wang,Yuanming Li,Shihan Zhang,Jianmeng Chen,Jingkai Zhao
The chemical absorption-bioelectrochemical reduction (CABER) integrated system provides an alternative of good potential for NO removal. The efficient utilization of cathode electrons directly determines the system performance and operating cost. Herein, we synthesize a polypyrrole/carbon nanotubes (PPy/CNTs) composite to engineer a micro-and nanoscale interface with low resistance and high biocompatibility between the cathode and biofilms in the CABER system. The resulting PPy/CNTs biocathodes exhibit 36.4% increase in biomass density, 40.7%–302.6% increase in Faraday efficiency along Fe(III)EDTA reduction, and 204% increase in Fe(II)EDTA-NO reduction rate. The enrichment of functional microorganisms is validated to be a key strengthening factor, as the proportion of which increased from 57.9% to 84.6%. Moreover, for efficient electron transfer and utilization, a low-resistance electron transfer route, “electrode substrate → PPy (→ CNTs) → microbial cells → Fe(III)EDTA or Fe(II)EDTA-NO”, is realized in the multiscale conductive networks constructed of PPy/CNTs composite and microbial nanowires .
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高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Xiaofei Miao,Qi Chen,Yongchuan Liu,Xiangxin Zhang,Yuanqiang Chen,Junhong Lin,Sujing Chen,Yining Zhang
At present, Zinc-iodine (Zn//I) batteries have attracted much attention due to their high safety and capacity. However, how to suppress the shuttling of polyiodide ions generated during charging processes is still a tricky problem. Herein, polyaniline (PANI) and polypyrrole (PPy) are electro-polymerized on carbon felt (CF) by constant current and used as cathodes for zinc-iodine (Zn//I) batteries. Electrochemical tests of the PANI@CF and PPy@CF electrodes prove that the PANI@CF electrode has a higher capacity, a stronger ability to suppress shuttling of polyiodine ions, and more excellent cyclic stability than the PPy@CF electrode. According to the material characterizations, the differences of both electrodes in electrochemical performances are mainly caused by the microstructures of PANI and PPy in both electrodes. The PANI has a micro-nano porous structure while the PPy is very dense. The porous PANI not only has more channels for the infiltration of electrolyte, but also can provide more active adsorption sites to minimize the shuttling of polyiodide ions to anode, ensuring the excellent performances of the PANI@CF. However, dense PPy seriously hinders the electrolyte diffusion and triggers the formation of an insulating dense iodine film, bringing poor performances to the PPy@CF. Ultimately, the PANI@CF electrodes achieves the most specific capacity of 235.9 mAh g −1 at 0.35 A g −1 (∼1.7 C) and performs out long cycle life with high stability (75.7% capacitiy rention after 10,000 cycles) at 3.5 A g −1 (∼17 C) in Zn//I battery , manifesting the porous PANI@CF electrode is a greatly promising candidate as cathode for Zn//I batteries in actual application.
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CELLULOSE
·
2022
·Vol. 29
·期 4
·2525-2537
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IF 6.123
Liang Chunliu,Zang Limin,Shi Fangfang,Yang Chao,Qiu Jianhui,Liu Qifan,Chen Zhenming
Cotton fabric (CF) fabricated by natural cellulose fibers has porous structure, abundant hydrophilic hydroxyl groups and good mechanical flexibility, which is a promising substrate for flexible fabric-based supercapacitors. Graphene oxide (GO) nanosheets were fixed on the CF by vacuum filtration, and then the pyrrole monomers and silver ions (Ag + ) were adsorbed to the surface of GO/CF by π-π and electrostatic interactions, respectively. Polypyrrole/silver (PPy/Ag) nanoparticles were generated on the surface of GO/CF via in situ UV-induced polymerization, forming the flexible PPy/Ag/GO/CF electrodes. The electrodes combine three active materials (PPy, Ag and GO), which show good electrochemical performance. The electrode prepared under optimum conditions (UV irradiation time: 120 min; mass loading of GO on the CF: 3 mg cm −2 ) exhibits a high specific capacitance of 1664.0 mF cm −2 . The flexible symmetric quasi-solid-state fabric-based supercapacitor (QFSC) based on the optimum electrode also keeps superior electrochemical performance and excellent mechanical flexibility, which has a great application prospect for wearable energy storage devices.
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DYES AND PIGMENTS
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2022
·
IF 5.122
Peiyu Tan,Feifei Lu,Yuge Han
A dual-layer structure combining the properties of two polymers is demonstrated to be efficient in strengthening the mid-to-far infrared modulation. Prior to the assembly of bilayer devices, the infrared adjustment capability of single-layer devices poly(3,4-ethylenedioxythiophene) ( PEDOT )、poly(pyrrole) ( PPY ) and poly(aniline) ( PANI ) with different polymerization charges is scrutinized. The results exhibit that the optimal polymerization charge affording the highest reflectance variation is inconsistent between the mid-wavelength and long-wavelength bands in PEDOT and PPY devices. However, through the arrangement of deposition sequence and relative thickness of PEDOT and PPY coatings, a device with the reflectance contrast of 0.662 in the mid-wavelength and 0.281 in the long-wavelength bands was obtained utilizing a bilayer film PEDOT-0.2C/PPY-0.3C . Further FTIR and UV–Vis spectra show that the bilayer films are successfully formed and both polymers play a role in the electrochemical process . Different morphologies of bilayer films with reverse positions observed by SEM images account for the correlation between the infrared regulation performance and deposition sequence.
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Reaction Chemistry & Engineering
·
2022
·Vol. 7
·期 4
·917-928
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IF 5.2
Tongxin Xiao,Ying Chen,Yuning Liang
The conversion of CO2 and water into valuable chemicals under sunlight irradiation is of great significance for solving the widespread problems of both limited energy sources and global warming. In this work, new artificial photosynthesis was established through a photocatalysis process of reducing CO2 to CH4. A photocatalyst compounded from a porphyrin (metalloporphyrin) and TiO2 nanotube arrays (TiO2NTs) was prepared, and its photocatalytic performance for CO2 reduction under Xe lamp irradiation was studied. Compared with the pure TiO2NTs, the photocatalytic CO2 reduction activity of metalloporphyrin-sensitized TiO2NTs is significantly enhanced. The amount of methane produced with the cobalt tetra(4-carboxyphenyl)porphyrin/TiO2NTs (CoTCPP/TiO2NTs) photocatalyst is about 5.5 times higher than that produced with TiO2NTs alone. The improvement of photocatalytic activity can be ascribed to the enhancement of light absorption ability of CoTCPP/TiO2NTs and the inhibition of electron–hole recombination. Furthermore, according to the results of the photocatalytic and photo(electro)chemical experiments, a probable mechanism for the photoreduction of CO2 over CoTCPP/TiO2NTs is presented.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Peng Lei,Ying Zhou,Bei Li,Yang Liu,Chuan Dong,Shaomin Shuang
The unique combination of DNA bases is essential for storing genetic information. A reliable and accurate electrochemical sensor based on a gold/palladium–polypyrrole/graphene nanocomposite (Au/Pd–PPy/GR) has been prepared to individually and simultaneously detect guanine (G), adenine (A), thymine (T), and cytosine (C). The bimetallic nanomaterial (Au/Pd–PPy) is used to enhance the sensing performance of DNA bases, and the GR could further increase the electroactive area and amplify the electrochemical response. As expected, the electrochemical sensor shows excellent electrocatalytic activity with well-separated current responses at 0.704 V (G), 0.976 (A), 1.164 (T), and 1.348 V (C). The prepared sensor exhibits the linear range of 1–350 μM for G, 5–300 μM for A, 20–900 μM for T, and 10–700 μM for C. The developed device is also demonstrated as an excellently sensitive and highly selective sensor to identify the four bases in calf thymus DNA, which provides the application of electrochemical sensors in bioscience.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 5
·2101877
·
IF 6.389
Chao Wang,Yuan Ha,Xin Mao,Weilan Xu,Aijun Du,Renbing Wu,Shulei Chou,Haijiao Zhang
The exploration of high-efficiency and inexpensive electrocatalysts for oxygen reduction reaction (ORR) is of critical significance for renewable energy conversion. Herein, an in situ catalytic transformation strategy toward a unique hierarchical nanostructure is reported. In the architecture, Co nanoparticles encapsulated at the tip of bamboo-like N-doped carbon nanotubes (NCNTs) are grafted on N-doped polypyrrole-derived CNTs. Thanks to the smart design of unique 3D architecture, the NPCN@Co-NCNTs catalyst displays an extraordinary ORR activity in 0.1 m KOH solution (the onset and half-wave potentials are 0.96 and 0.90 V vs RHE, respectively), which is similar to commercial Pt/C catalyst (0.99 and 0.88 V vs RHE, respectively). Meanwhile, the catalyst shows the low Tafel slope of 78 mV dec −1 and long-time stability. Experimental and theoretical results verify that the improved ORR performance is mainly related to the existence of Co nanoparticles protected by pyridinic-N-doped carbon, which lowers the theoretical overpotential of ORR. Density functional theory calculations reveal that Pyridinic-NC Co site is the reactive site with the lowest overpotential for ORR (0.57 V). These results unambiguously indicate that the NPCN@Co-NCNTs represent a low-cost yet high-efficiency electrocatalyst for the electrocatalytic ORR.
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Molecular Catalysis
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2022
·
IF 5.089
Yongjian Qiu,Yaju Chen,Lin Lei,Xilun Wang,Xiaojing Zeng,Zhengfeng Feng,Chunyan Deng,Dongying Lin,Hongbing Ji
Porphyrin-bearing porous materials have attracted great interest in the field of CO 2 chemical fixation, yet one-pot fabricating networks with multifunctionality through bottom-up oriented synthetic method is still scarce and balancing the multifunction and the porosity remains challenging. Herein, we designed an ionic liquid-based building unit with rigidity and contortion and then synthesized a porous ionic polymers (PiPs) consisting of electrophilic metalloporphyrin and nucleophilic imidazolium ionic liquids (ILs) units by “Adler-Longo” methodology and metallization reaction. The as-prepared bifunctional polymer ZnPor-PiP possessed improved specific surface area, abundant micro/mesoporosity, noteworthy CO 2 uptake and acceptable CO 2 /N 2 selectivity. Legitimately, ZnPor-PiP exhibited good catalytic performance for the synthesis of cyclic carbonates from CO 2 and epoxides under mild conditions owning to the cooperative effect between the metal active center and the IL moieties, as well as the unique structural properties. Intriguingly, ZnPor-PiP gave a good substrate expansibility for this cycloaddition reaction and showed no obvious decrease in catalytic activity over six recycles. Furthermore, this bifunctional solid catalyst could efficiently convert diluted CO 2 (15% CO 2 in N 2 ) with propylene epoxide into propylene carbonate at 100 °C and 3.0 MPa. This bottom-up oriented strategy is of great importance for the development of functionalized porphyrin-based PiPs and the as-designed polymers highlights the potential for targeting CO 2 capture and transformations.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 29
·44845-44861
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IF 5.19
Wang Jiangyuan,Yu Qiu,Zheng Yi,Li Jing,Jiao Binquan,Li Dongwei
Toxic metal pollutant Cr(VI) in the environment will pose a severe threat to animal and human health. In this work, Fe 3 O 4 @PPy, Arg@PPy, and Arg/Fe 3 O 4 @PPy were prepared to enhance adsorption of Cr(VI) by doping Fe 3 O 4 nanoparticles and amino radicals into the original PPy structure. Their characteristics were investigated by FTIR, SEM, EDS, BET analysis, and batch adsorption experiments. And they were used as permeable reaction barriers (PRB) to combine with electrokinetic remediation (EKR) to remediate Cr-contaminated soil. Adsorption experiment results showed that the maximum adsorption capacities of PPy, Fe 3 O 4 @PPy, Arg@PPy, and Arg/Fe 3 O 4 @PPy for Cr(VI) were 60.43 mg/g, 67.12 mg/g, 159.86 mg/g, and 141.50 mg/g, respectively. They all followed the kinetic pseudo-second-order model and the Langmuir isothermal model with a monolayer adsorption behavior. In the EKR/PRB system, the presence of Fe 3 O 4 @PPy, Arg@PPy, and Arg/Fe 3 O 4 @PPy obtained the higher Cr(VI) removal efficiency near the anode than that of the PPy, increasing by 74.60%, 26.04%, and 68.64%, respectively. A strong electrostatic attraction between anion contaminants and protonated modified PPy and a reduction from Cr(VI) to Cr(III) appeared in the EKR remediation process under acid conditions. This study opened up a prospect for applying modified PPy composites to treat toxic metal-contaminated soil.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Min Wang,Guorong Xu,Zihan An,Ke Xu,Chunhua Qi,Rasel Das,Heli Zhao
Solar vapor generation (SVG) has emerged as a promising technique of harvesting solar energy for producing fresh water from seawater. However, two main problems of insufficient energy utilization and salt accumulation on evaporation surfaces are still challenging issues for the broad application of this technique. In this work, we demonstrate a hierarchically structured bilayer aerogel by in situ deposition of polypyrrole (PPy) inside the top layer of cellulose . The light-absorbing PPy/cellulose composite with three-dimensional (3D) hierarchical structures served to convert solar energy into thermal energy and localize the heat to power the vaporization of water contained in the cellulose network. While the porous and hydrophilic cellulose matrix enabled continuous water transport and replenishment to the upper evaporative layer. Moreover, several microcracks were formed at the PPy/cellulose surface, which assisted vapor escape and salt re-dissolution. As a result, the prepared PPy/cellulose aerogel enabled a high seawater evaporation rate of 1.42 kg m −2 h −1 at energy efficiency of 97.8% under one sun illumination. The SVG system also exhibited highly efficient and stable evaporation performance in seawater without surface salt accumulation over one week.
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Energy & Environmental Materials
·
2022
·Vol. 6
·期 3
·e12353
·
IF 13.443
Boqiu Luo,Jin Wen,Hao Wang,Size Zheng,Rui Liao,Wenjing Chen,Omid Mahian,Xiaoke Li
Solar-driven hydrogel evaporator used for water purification demonstrates great potential in seawater desalination and domestic sewage treatment. However, much uncertainty still exists about the most efficient design to obtain cost-effective drinkable water. In this paper, a natural rich biomass Nicandra physalodes (Linn.) Gaertn. polysaccharide was introduced into the polyvinyl alcohol network to control the water distribution during evaporation and build a low-cost hybrid hydrogel solar evaporator with a total material cost of $7.95 m −2 . The mixed evaporator works stably in a long-span acid–base range (pH 1–14) and salinity range (0–320 g kg −1 ). Its daily water purification capacity can reach 24.4 kg m −2 with a water purification capacity of 3.51 kg m −2 h −1 under sunlight. This paper provides a new possibility for a highly efficient and cost-effective water desalination system with guaranteed water quality by focusing on the dynamic regulation of water molecules at the evaporation interface.
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Environmental Science-Nano
·
2022
·Vol. 9
·期 3
·1091-1105
·
IF 9.473
Heng Shi,Yi He,Yubin Li,Teng He,Pingya Luo
Metal–organic frameworks (MOFs) for persulfate-based Fenton-like processes have attracted tremendous attention nowadays. However, the low utilization of active sites and poor stability of MOFs still impede their practical application. In this work, we demonstrate a unique photo Fenton-like catalyst with confined ultrasmall MOF nanoparticles anchored on a 3D-graphene network, which is fabricated through a simple confined thermal pulverization method. The ultrasmall Co–Fe MOF nanoparticles with confined structure endowed this catalyst with highly exposed active sites as well as excellent stability. It can maintain high degradation efficiency via visible light-assisted peroxymonosulfate (PMS) activation in a broad pH range from 1–13. Electron spin resonance (ESR) technology reveals that both radical and nonradical processes are involved in this process, and the broad pH adaptability of this system is due to the stable generation of ˙OH, SO4˙−, ˙O2−, and 1O2 under these pH conditions. This study provides new perspectives for the development of highly efficient and harsh environment-adaptive MOF-based Fenton-like catalysts.
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