JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Qi Xia,Jinlong Hu,Qingqing Chen,Lingzhi Zhang
Selenium cathode attracts great attention due to its high theoretical volumetric capacity and better electrical conductivity than sulfur cathode. Herein, N/S co-doped microporous carbon (NS-K-PC) is designed and prepared as Se host by a spray drying process of the poly(styrenesulfonic acid)-melamine salt solution followed by carbonization and activation process. The as-prepared NS-K-PC shows a very high micropore contribution of 94.8% in the total surface area, and a total N/S heteroatom doping level of 2.5 wt% in the carbon matrix. The NS-K-PC/Se cathode delivers a high reversible capacity of 499.2 mA h g −1 at 0.1C, superior rate capacity of 324 mA h g −1 at 8C, and great cycling stability with a capacity decay of 0.081% per cycle over 500 cycles at 1C. Additionally, a comparative study demonstrates that NS-K-PC/Se cathode with the carbonate-based electrolytes exhibit better cycling stability than those with ether-based electrolytes primarily resulted from a direct solid–solid conversion of Se to Li 2 Se bypassing the formation of soluble polyselenides.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Huicai Zheng,Guichuan Xu,Wen Li,Xiaoju Zhang,Binshen Wang,Li Qin,Limei Zhou
Here we report a strategy to synthesize efficient polymeric carbon nitrides/3D honeycomb poly(ionic liquid)s photoreactor. The initial parent polymeric carbon nitrides (PCN) were synthesized by sintering precursor formed by self-assembling molecules of cyanuric acid and melamine. Ionic liquids with polymerizable groups polymerized in situ with crosslinkers in a system dispersed in PCN to synthesize a photoreactor. Impressively, the obtained photoreactors have structurally stable nanoparticle morphology in a dry state and a transparent 3D network structure in a swelling state. Their successful formation, swelling ability and morphology were fully characterized by XRD, WAXS, FT-IR, SEM, XPS, TEM and N 2 adsorption/desorption isotherm. UV–vis DRS, PL spectra, and photocurrent tests showed the improved photo-electric property of the photoreactor, which was attributed to the 3D network honeycomb structure improving the contact between the active centres in the reactor and the reaction substrate and the improving electron-hole separation efficiency of PCN by excellent electron transfer ability of poly(ionic liquid)s. These synthesized photoreactors could highly efficiently degrade the anionic dyes, such as methyl orange and acid blue 93, under a metal halide lamp or even natural sunlight.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2023
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IF 3.3
Zehui Liu,Dianjin Ding,Jinzhao Huang,Jun Tang,Sixuan Zhang,Xiaolong Deng
It's still a challenge to design reasonably efficient catalyst using non-noble metal for the oxygen evolution reaction (OER). In this paper, we use a simple one-step electrodeposition method to load Ce and S co-doped NiFe amorphous alloys onto Cu(OH) 2 nanorod arrays. The excellent oxygen electrocatalytic performance of the catalyst NiFeCeS/Cu(OH) 2 /CuF is attributed to the electronic environments of the active sites of Ni and Fe regulated by heteroatomic sulfur and cerium , which promote the transfer of the oxygen precipitation intermediates to the higher valence states. Meanwhile, the highly conductive substrate accelerates the electron transfer efficiency of the catalyst material, and the loose nanostructure increases the specific surface area , exposing more active sites. NiFeCeS/Cu(OH) 2 /CuF shows outsanding electrocatalytic activity for oxygen evolution with a low overpotential of 227 mV at a current density of 10 mA cm −2 in alkaline medium. Moreover, the nanocomposite catalyst also exhibits rapid reaction kinetics and long-term stability and durability. In this work, an efficient oxygen precipitation catalyst is reported, which indicates that non-precious metal-based electrocatalysts have great potential for application in water electrolysis and provides a basis for the rational design and synthesis of nanorod array catalysts with unique structures.
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ACS Applied Nano Materials
·
2023
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IF 5.9
Yingsha Wang,Qinghua Feng,Meili Liu,Liuheng Xue,Gang Wang,Shouting Zhang,Wenping Hu
Developing peroxidase-like sensors with excellent catalytic activity to construct colorimetric sensors has been an important challenge for a long time. The electronegativity of the doped nonmetallic atoms can change the chemical environment of the carbon material and promote the redistribution of electrons, thus improving the electron transfer channel between the nanozyme and the reaction substrate and further enhancing the peroxidase-like activity. Herein, a nitrogen (N), phosphorus (P), and sulfur (S) codoped carbon nanozyme (NPS-C) was successfully designed via one-step high-temperature pyrolysis. Compared with N-doped nanozymes (N–C), N and P codoped carbon nanozymes (NP-C) have a lower Michaelis–Menten constant, and N and S codoped carbon nanozymes (NS-C) have a higher reaction rate. Therefore, based on the synergy between different atoms, NPS-C exhibited excellent peroxidase-like activity and stronger substrate binding affinity, which effectively activated H2O2 to produce reactive oxygen intermediates with a stronger oxidation capacity and superoxide anion radical (•O2–) and promoted TMB to lose an electron and be oxidized to oxTMB. Moreover, ascorbic acid (AA), as an antioxidant model, can rapidly consume reactive oxygen species and reduce oxTMB. Therefore, based on the excellent peroxidase-like activity of NPS-C and the linear relationship between the concentration of AA and the inhibition degree of peroxidase-like activity, a colorimetric sensor can be constructed to analyze the total antioxidant capacity (TAC) in beverages.
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JOURNAL OF POWER SOURCES
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2023
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IF 9.2
Yunji Xie,Kaiqi Wang,Di Liu,Jinhui Pang
Concentrated functionalization of the polymer side chain is widely considered as an effective structural strategy for improving the properties of anion exchange membranes (AEMs). However, the synthetic process typically involves highly toxic reagents. Herein, a series of poly(arylene ether ketone)s with densely benzyl- N -methylpiperidinium-functionalized hexaphenylbenzene pendants is synthesized, avoiding the demand of highly toxic reagents. The fabricated membranes present pronounced microphase separation resulting from the strong contrast in polarity between the hydrophobic polymer backbone and hydrophilic pendants. In contrast to analogous AEMs, the incorporation of bulky and rigid hexaphenylbenzene moieties enlarges the free volume within the membranes, which significantly enhances water absorption and inhibits dimensional change. Moreover, the presence of piperidinium-based cationic groups considerably enhances the alkaline stability of the membranes. One of the prepared membranes with an ion exchange capacity of 1.31 meq g −1 exhibits water uptake, swelling ratio, and hydroxide conductivity of 67.2%, 14.5%, and 49.2 mS cm −1 at 80 °C, respectively. The loss of conductivity is less than 6% after immersion in a 4 M KOH aqueous solution at 30 °C for 480 h. Additionally, a maximum power density of 340.1 mW cm −2 is achieved in the H 2 /O 2 single-cell test, indicating promising application potential for the fabricated membranes.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 45
·16773-16779
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IF 4
Mincong Liu,Jing Zhang,Guohua Ye,Yan Peng,Shiyou Guan
Zn–N–C catalysts have garnered attention as potential electrocatalysts for the oxygen reduction reaction (ORR). However, their intrinsic limitations, including poor activity and a low density of active sites, continue to hinder their electrocatalytic performance. In this study, we have devised a dual-template strategy for the synthesis of Zn, N, S co-doped nanoporous carbon-based catalysts (Zn–N/S–C(S, Z)) with a substantial specific surface area and a graded pore structure. The introduction of S enhances electron localization around the Zn–Nx active centers, facilitating interactions with oxygen-containing substances. The resulting Zn–N/S–C(S, Z) sample exhibits outstanding performance in an alkaline solution, demonstrating a half-wave potential of 0.89 V. This value surpasses that of commercial Pt/C by 40 mV. Furthermore, when combined with RuO2 (Zn–N/S–C(S, Z) + RuO2), the catalyst demonstrates exceptional performance in a Zn–air battery, offering an open-circuit voltage (OCV) of 1.47 V and a peak power density of 290.8 mW cm−2. This study paves the way for the development of highly dispersed and highly active Zn-metal site catalysts, potentially replacing traditional Pt-based catalysts in various electrochemical devices.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Jing Zhang,Xingjie Shang,Ying Zhu,Xuan Yang,Shu Wang,Feixiang Gong,Lei Wang,Hongpeng Ma
To explore the intrinsic correlation between the rigidity and distortion degree of polymer backbones and the diffusion dialysis (DD) performance of anion exchange membranes (AEMs), pyrrolidinium-functionalized poly(arylene ether sulfone)s containing different Cardo (TPM) moieties were prepared. The structures, properties and DD performance of above AEMs were systematically evaluated. As the Cardo (TPM) group angle increased, the d-spacing, fractional free volume, and membrane area resistance increased, and the microphase separation structures, hydrophilicity, and acid flux decreased, mainly because larger Cardo (TPM) group angles are unfavourable for the close packing of polymer chains in space. Both the Cardo-type and TPM-type AEMs exhibited universal ultrahigh H + /Fe 2+ selectivity (S > 3819), which was mainly attributed to the synergistic influence of their rigid narrow ion transport channels, small pore diameter (0.48–0.62 nm) and narrow pore size distribution (0.24–0.68 Å). Additionally, due to the high-density amide groups of TPM units, which decreased the hydrophobicity of the polymer skeleton and induced the formation of an additional transport pathway for Fe 2+ through hydrogen bonding interactions, the TPM-type AEMs showed both lower acid flux and selectivity, suggesting that the structure of hydrophilic auxiliary groups should be carefully designed when improving the DD performance of AEMs.
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FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Ke Li,Mengxia Yan,Haili Wang,Lifen Cai,Ping Wang,Huimin Chen
As a typical high-efficient alkane aromatization catalyst, Pt/KL is prone to deactivation due to the sintering growth of Pt on the outer surface of KL and the channel blockage caused by carbon deposition , which is further exacerbated by the one-dimensional channel structure of KL. Therefore, a series of encapsulated catalysts combining the three-dimensional channel structure advantages of S-1 with the role of potassium are prepared and evaluated. It is shown that the encapsulated catalyst KPt@S-1-02 modified by moderate potassium exhibits extremely superior stability and no significant deactivation is observable after n-heptane aromatization for 180 h under harsh conditions. On the one hand, encapsulation structure enables a strong anti-agglomeration ability of Pt and the topological structure of S-1 endows the encapsulation catalysts less susceptible to channel blockage, which has been demonstrated by HAADF-STEM and N 2 -adsorption. On the other hand, characterizations involving NH 3 -TPD, CO-DRIFT and HAADF-STEM verify that the modification by an appropriate amount of K can inhibit acid sites of catalysts and improve Pt dispersion and electron density, thus enhance the stability of catalysts. However, excessive K can serve as weak acid sites, poison of active sites and inhibitor of H 2 adsorption on Pt surface, leading to deactivation of the catalyst.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Qian Wang,Limei Sheng,Xuan Guo,Rong Chen,Chengjie Zhou,Fu Yang
Dynamic kinetic resolution (DKR) of chiral amines with enzyme and noble metal has been widely concerned in chemistry, biology and pharmacy fields. While the synergistic effect and long-term stability of enzyme-noble metal in catalysts remain challenging. In this paper, several functional polymers were designed and employed as the carrier of lipase and palladium (Pd) for one-pot DKR of α-phenethylamine. By modulating the multisite weak force (MSWF) of the polymers on the active centers, the optically pure product with high conversion (>99%) and ee (>99%) were obtained and the designed catalyst Pd@PE-2OH_CalB showed superior stability to other commercial catalysts, such as Pd/C and Novozym 435. Additionally, the heterogeneous chemoenzymatic catalysts could be easily recovered and recycled up to seven times without sacrificing efficiency. Further investigation revealed that the enhanced catalytic performance depended on MSWF formed by the abundant ionic sites, functional groups, and lots of hydrogen bonds of poly(ionic liquid)s.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Mingming Song,Xianghai Song,Xin Liu,Weiqiang Zhou,Pengwei Huo
The design of a heterogeneous structure for photocatalysts has attracted significant attention. In this study, a step-scheme (S-scheme) heterojunction was designed using an in-situ synthesis method. The resulting heterojunction comprised 3D microspheres of ZnIn 2 S 4 and octahedral MOF-808 (ZnIn 2 S 4 /MOF-808). During this process, we investigated the impact of the scale of the ZnIn 2 S 4 microspheres on performance by controlling the growth of the ZnIn 2 S 4 microspheres with various scales. The maximum catalytic activity was discovered to be achieved with ZnIn 2 S 4 microspheres of 6 µm when coupled with MOF-808. Compared to pure ZnIn 2 S 4 and MOF-808, the fabricated S-scheme ZnIn 2 S 4 /MOF-808 heterojunction exhibited notably improved photocatalytic CO 2 reduction performance. The performance of the CO yield of the optimized sample could reach 8.21 μmol g −1 h −1 , which was approximately 10 and 8 times higher than those of ZnIn 2 S 4 (0.84 μmol g −1 h −1 ) and MOF-808 (1.03 μmol g −1 h −1 ), respectively. Moreover, ultraviolet photoelectron spectroscopy, ESR, in situ X-ray photoelectron spectroscopy, and density functional theory calculations were used to study the charge transfer mechanism of the S-scheme heterojunction. In-situ FT-IR investigation established the Carbene pathway as the source of CO production (CO 2 → CO 2 * → COOH* → CO* → CO). This study provides an efficient method for designing an S-scheme heterojunction for photocatalytic CO 2 reduction.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xiaoqian Peng,Yingyi Li,Kairuo Zhu,Qingda An,Jingai Hao,Zuoyi Xiao,Xiaoling Dong,Shangru Zhai
Exploiting low-cost and high-performance biochar catalysts is vital for the detoxification of organic wastewater and the resource utilization of algal biomass. Herein, CoS x containing biochar (CoSBC) was prepared using exogenous Co salt and endogenous Porphyra rich in S elements for enhanced degradation of carbamazepine (CBZ) by peroxymonosulfate (PMS) activation. 95.73% of CBZ (20 mg/L) can be removed within 20 min in CoSBC-900/PMS system with a degradation rate of 0.1287 min −1 , and maintained a higher catalytic efficiency after five cycles (> 90%). Besides, the CoSBC-900/PMS system held excellent resistance over various coexisting substances, and could efficiently degrade multiple organic contaminants . Mechanism analyses revealed that 1 O 2 and SO 4 •− collaborated for CBZ degradation, in which 1 O 2 played the dominant role and 1 O 2 mainly originated from the formation process: PMS→O 2 •− → 1 O 2 . The low redox potential of S species accelerated Co(II)/Co(III) circulation, while Porphyra biochar also served as the highly active centers, producing abundant active species (SO 4 •− ). The possible intermediate products accompanying CBZ degradation were proposed based on LC-MS analysis and the corresponding toxicity assessment verified that the CoSBC-900/PMS system possesses desirable CBZ detoxification ability. This study provides novel insight into the development of transition metal-based biochar catalysts from algal biomass for the purification of organic wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaoyan Ding,Yanjun Xue,Jingjing Wang,Jian Tian
Heterojunction engineering is an effective strategy to improve photocatalytic performance. Two-dimensional (2D)/2D semimetal 1T′ phase molybdenum sulfide/zinc indium sulfide (1T′-MoS 2 /ZnIn 2 S 4 ) S-scheme heterojunctions with tight and stable interfaces were synthesized by a simple hydrothermal synthesis method. Under the optimal 1T′-MoS 2 loading ratio (5 wt%), the hydrogen production rate of 1T′-MoS 2 /ZnIn 2 S 4 composites reaches 11.42 mmol h −1 g −1 , which is 3.1 and 1.4 times higher than that of pure ZnIn 2 S 4 (2.9 mmol h −1 g −1 ) and ZnIn 2 S 4 /Pt (8.01 mmol h −1 g −1 ), and the apparent quantum efficiency (AQE) reaches 53.17 % (λ = 370 nm). Semimetal 1T′ phase MoS 2 on ZnIn 2 S 4 broadens the light absorption range, enhances the light absorption ability, promotes electron transfer, and offers abundant active sites. The establishment of S-scheme heterojunctions achieves the spatial separation of photogenerated charges and increases the reduction potential. This work provides insights for the design of novel photocatalysts.
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