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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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 4
·1084-1093
·
IF 6.813
Meilian Gao,Pingping Gao,Ting Lei,Chun Ouyang,Xiaobo Wu,Anru Wu
A novel porous iron phosphide (p-FeP) loading on nitrogen-doped carbon fiber/carbon paper (p-FeP/NCF/CP) as highly effective self-supporting catalysts for the hydrogen evolution reaction (HER) is synthesized by a three-step approach, including N-doped carbon fiber network preparation, porous FeOOH/NCF/CP precursor by selectively etching, and subsequent phosphorization process. The as-obtained p-FeP/NCF/CP composite exhibits a higher specific surface area and larger porosity in comparison to FeP/CP composite due to the rich porous structure and 3D network of the N-doped carbon fiber matrix (NCF). Electrochemical measurements demonstrate that p-FeP/NCF/CP composite exhibits an excellent electrocatalytic activity for HER with small overpotentials of 63 mV and 96 mV at 10 mA cm−2 current density in 0.5 M H2SO4 and 1.0 M KOH, respectively. The p-FeP/NCF/CP material also exhibits a small Tafel slope and charge transfer resistance as well as good stability and durability in pH 7 and pH 14.
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POLYMER
·
2022
·
IF 4.432
Junping Lv,Lin Zhu,Meng Zhang,Zexu Zhao,Shu-Wei Chen,Jinyi Wang
Actuators with controllable and reversible morphing towards environment stimuli have great potential applications in diverse fields. In spite of good progress made over the past decades, simple and efficient preparation of multi-response actuators is still a challenge. Here, we report a strategy to prepare humidity and near infrared (NIR) dual-response actuators with controllable and reversible bending or twisting deformation. The actuators were made up of two layers, one was polyvinyl butyral (PVB) layer with humidity and NIR inertness, and the other was chlorine-modified polypyrrole (PPy-Cl) doped poly(N-isopropylacrylamide-co-benzophenone) (PNIPAM-ABP) composite layer, taking advantage of the NIR photothermal conversion capability of PPy-Cl, along with the thermal-responsive PNIPAM-ABP. Upon NIR light irradiation , PPy-Cl converted light energy into heat, which subsequently induced the shrinkage of poly(N-isopropylacrylamide) (PNIPAM) chains; upon a high-humidity environment, PPy-Cl absorbed water molecular and transferred it into PNIPAM polymer , which further caused the bilayer to shrink or swell in an asymmetric manner, consequently leading to reversible bending or unbending behaviors. Interestingly, upon ultraviolet (UV) light irradiation with a grid photomask, the bilayer actuators showed bending or twist behaviors along with a special direction. The bionic flowers made from the actuators could imitate sunflower's opening and closing behaviors in response to NIR or humidity. The dual-response actuator could also imitate the lifting weight behaviors of forklifts. As an interesting example for potential utilization, a smart four-wheel vehicle was constructed using the bilayer actuator, showed excellent fast-moving performance.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2022
·
IF 9.879
Yanqin Wang,Jingwen Liao,Xiaogang Wu,Fengbo Zhu,Yang Liu,Yi-Xian Qin,Weiyi Chen,Qiang Zheng
Flexible switching devices with multi-stimulus responsive abilities have shown promising applications as smart materials in the tissue regeneration fields. Herein, a composite hydrogel-based flexible switch system was successfully designed by integrating the nano-sized conductive CNC@PPy (cellulose nanocrystal decorated with polypyrrole (PPy)) and CNC@PDA (cellulose nanocrystal decorated with polydopamine (PDA)) composite particles into the thermal sensitive poly N-isopropyl acrylamide (PNIPAM) hydrogels. The resulting composite hydrogels exhibited enhanced elastic modulus (∼29.5 kPa), superior conductivity (∼1.1 S/m), self-healing, and thermo- and NIR-responsive abilities. Particularly, the incorporated CNC@PDA and CNC@PPy particles within the hydrogel matrix by hydrogen bonds could not only provide a more continuous transporting path for electrons, but also further improve the photothermal conversion efficiency of the composite hydrogel system, in which the temperature increased by 47.6 °C within 10 min under NIR irradiation, and high NIR light-responsive sensitivity with a volume change of 30% within 2 min. Moreover, these composite hydrogels were developed to serve thermo- and NIR light-responsive switchers effectively, which showed excellent stimulus-responsive sensitivities. In all, this work provided a new strategy for designing the multi-stimulus responsive smart hydrogels, which demonstrated excellent potential to serve as remotely controllable switch devices in biomaterials and tissue regeneration.
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ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200090
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IF 9.14
Wenwen Bao,Senhe Huang,Diana Tranca,Boxu Feng,Feng Qiu,Fermín Rodríguez-Hernández,Changchun Ke,Sheng Han,Xiaodong Zhuang
Graphical Beauty in balanced asymmetry : An asymmetric Co II porphyrin ( as -PorCo) is constructed with a substituent of 2,6-dimethylbenzene to enhance the charge transfer capability from carbon nanotubes to as -PorCo, resulting in large partial current density of 8 mA cm −2 and high turnover frequency of 5656 h −1 at −0.7 V vs. reversible hydrogen electrode in aqueous solution. The present study provides the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction. The electrochemical reduction of carbon dioxide (CO 2 ) based on molecular catalysts has attracted more attention, owing to their well-defined active sites and rational structural design. Metal porphyrins (PorMs) have the extended π-conjugated backbone with different transition metals, endowing them with unique CO 2 reduction properties. However, few works focus on the investigation of symmetric architecture of PorMs as well as their aggregation behavior to CO 2 reduction. In this work, a series of Co II porphyrins (PorCos) with symmetric and asymmetric substituents were used as model of molecular catalysts for CO 2 reduction. Owing to the electron donating effect of 2,6-dimethylbenzene (DMB), bandgaps of the complexes became narrower with the increasing number of DMB. As electrocatalysts, all PorCos exhibited promising electrocatalytic CO 2 reduction performance. Among the three molecules, asymmetric Co II porphyrin ( as -PorCo) showed the lowest onset potential of −288 mV and faradaic efficiencies exceeding 93 % at −0.6 V vs. reversible hydrogen electrode, which is highly competitive among the reported state-of-art porphyrin-based electrocatalysts. The CO 2 reduction performance depended on π-π stacking between PorCo with carbon nanotubes (CNTs) and adjacent PorCos, which could be readily controlled by atomically positioned DMB in PorCo. Density functional theory calculations also suggested that the charge density between PorCo and CNT was highest due to the weak steric hindrance in as -PorCo, providing the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction.
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Journal of Energy Storage
·
2022
·
IF 8.907
Qinzheng Hu,Shuzhen Cui,Kanjun Sun,Xiuting Shi,Mingxin Zhang,Hui Peng,Guofu Ma
Hydrogel electrolyte have multifunctional properties in the flexible supercapacitors, which can have excellent mechanical behavior and wide temperature tolerance. However, the hydrogel electrolytes with poor mechanical properties, unsatisfactory ionic conductivity and narrow temperature range are still a huge challenge to limit their widely use in the flexible supercapacitors. Herein, a novel ethylene glycol-containing polyacrylamide/montmorillonite/ionic liquid (EG-PAM/MMT/EMIMBF 4 , EG-PME) hydrogel with significant stretchability, high ionic conductivity and wide temperature tolerant was synthesized by a cross-linking polymerization process. The double-network structure can improve the mechanical properties of hydrogel. Moreover, the introduction of EG and EMIMBF 4 into the hydrogel can improve the temperature range. Furthermore, an integrated flexible supercapacitor with wide temperature range was fabricated by in-situ polymerization polypyrrole electrodes onto hydrogel. The integrated flexible supercapacitors have superior toughness under different mechanical deformation (e.g., stretch, compression and twisting ). The EG-PME-PPy composite film possesses high single electrode areal capacitance of 212 mF cm −2 at 0.8 mA cm −2 , high energy density of 9.4 μWh cm −2 at power density of 319.5 μW cm −2 , and good ionic conductivity of 5.18 mS cm −1 at -30 °C, as well as high ionic conductivity of 33.3 mS cm −1 at 40 °C. The integrated flexible supercapacitors have the satisfying electrochemical properties due to the rapid ion diffusivity and low charge transfer resistance of the integrated all-in-one hydrogel. Therefore, the developed all-in-one flexible supercapacitor based on multifunctional hydrogel can be a next-generation promising power sources.
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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Chaohu Xiao,Qimeige Hasi,Shanshan Wang,Yuhan Zhang,Hailing Li,Lu Zhang,Lihua Chen,An Li
Solar steam generation (SSG) is one of the promising technologies for seawater desalination and contaminated water purification . However, SSG devices are always restricted by poor insulation performance, insufficient solar spectrum absorption and serious salt-fouling. Here, a double-layered novel SSG system was fabricated by using poly(ionicliquid)s gels with hollow SiO 2 microspheres in-situ doping to enhance the thermal insulation of lower layer, and co-modified the top surface by polypyrrole (PPy) and silver particles to strengthen the solar absorption capability. Benefiting from the low thermal conductivity (0.082 W m −1 k −1 ), strong light absorption ( ca . 96%) and adequate water transport capability of poly(ionic liquid)s gels. As SSG device, a superb photothermal conversion efficiency of 90.5% is achieved under 1 sun illumination. Moreover, the poly(ionic liquid)s gels based SSG system also shows good desalination performance in artificial sea water and high concentration brine, and the purified water from artificial seawater can achieve the WHO's standard for drinking water . Therefore, this work combined attractive in-situ doping and co-modified strategies for fabricating high performance and thus shows significant potential for real applications.
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DYES AND PIGMENTS
·
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
·
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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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Jun Wan,Rong Hu,Junfeng Li,Shiyun Mi,Jinglin Xian,Zhiheng Xiao,Ziyang Liu,Aojie Mei,Siqi Xu,Mingzhao Fan,Huiyu Jiang,Qian Zhang,Huihong Liu,Weilin Xu
Conductive polymer (CP) fabric is considered as the ideal electrode for flexible energy storage due to its light weight, good flexibility and high energy storage properties. However, the conventional polymer-coated cellulose fiber synthesized by liquid-phase oxidation polymerization always forms disordered assembly of polymer particles on fiber, which endures poor mechanical stability. Here, we report a two-dimensional (2D) CP based fabric electrode realized by a salt-template assisted vapor-phase polymerization method, which achieves robust coating of 2D CP on various cellulose fibers. Typically, the prepared 2D polypyrrole@cotton electrode displays a high specific capacitance (902.6 mF cm −2 ) and good cycling stability (86.5% capacitance retention after 12,000 cycles). The capacitance of flexible symmetrical device retains at more than 90% when it is bent to 180° after 1000 bending cycles. This work provides a new strategy for the robust interface between functional materials and cellulose fibers, and has great potential for commercial mass production.
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