Journal of Environmental Sciences
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2022
·
IF 6.796
Yunlong Chen,Yingping Huang,Hailin Tian,Liqun Ye,Ruiping Li,Chuncheng Chen,Zhongxu Dai,Di Huang
With increasing concerns on the environment and human health, the degradation of glyphosate through the formation of less toxic intermediates is of great importance. Among the developed methods for the degradation of glyphosate, photodegradation is a clean and efficient strategy. In this work, we report a new photocatalyst by doping F ion on BiVO 4 that can efficiently degrade glyphosate and reduce the toxic emissions of aminomethylphosphonic acid (AMPA) through the selective (P)−C−N cleavage in comparison of BiVO 4 catalyst. The results demonstrate that the best suppression of AMPA formation was achieved by the catalyst of 0.3F@BiVO 4 at pH = 9 (AMPA formation below 10%). In situ attenuated total reflectance Fourier transforms infrared (ATR-FTIR) spectroscopy indicates that the adsorption sites of glyphosate on BiVO 4 and 0.3F@BiVO 4 are altered due to the difference in electrostatic interactions. Such an absorption alteration leads to the preferential cleavage of the C−N bond on the N−C−P skeleton, thereby inhibiting the formation of toxic AMPA. These results improve our understanding of the photodegradation process of glyphosate catalyzed by BiVO 4 -based catalysts and pave a safe way for abiotic degradation of glyphosate.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Jingsheng Zhou,Beibei An,Zhiyong Zhu,Li Wang,Jinglai Zhang
Doping heteroatoms in carbon materials is a promising method to prepare the robust electrocatalysts for the carbon dioxide reduction reaction (CO2RR), which is beneficial for sustainable energy storage and environmental remediation. However, the obscure recognition of active sites is the obstacle for further development of high-efficiency electrocatalysts, especially for the N,P-codoped carbon materials. Herein, a series of N,P-codoped carbon materials (CNP) is prepared with different N and P contents to explore the relationship between the N/P configuration and the CO2RR activity. As compared with the N-doped carbon materials, the additional P doping is helpful to improve the activity. The optimum N,P-codoped carbon materials (CNP-900) achieve 80.8% CO Faradaic efficiency (FECO) at a mild overpotential of 0.44 V. On the basis of the X-ray photoelectron spectroscopy results, the suitable ratio between pyridinic N and graphitic N and the least P–N content are beneficial for CO2RR. The density functional theory calculations further illustrate that two elementary steps to form *COOH and *CO in CO2RR are determined by the graphitic N and pyridinic N configurations, respectively. The existence of the P–N configuration breaks the equilibrium between graphitic N and pyridinic N to suppress the activity.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Wenming Fu,Yangzheng Huang,Luyao Deng,Jiahao Sun,Shao-Lu Li,Yunxia Hu
Organic solvent nanofiltration (OSN) is a green, environmentally friendly and sustainable separation technology. High-performance OSN membranes are expected to play a critical role in the field of chemical separation involving organic solvents. However, traditional OSN membranes suffer from the constraints on perm-selectivity. Herein, we introduced macrocyclic molecules with intrinsic angstrom-size cavity, pillar[n]arene (P[n]a, n = 5, 6), as a novel aqueous monomer to react with trimesoyl chloride (TMC) to prepare highly perm-selective thin-film composite (TFC) OSN membranes through interfacial polymerization. The prepared TFC-P[n]a membranes exhibit ultra-thin selective layer thickness of sub-10 nm and possess permanent intrinsic microporous structure, which endows the membrane with high perm-selectivity. Especially, the TFC-P[6]a membrane exhibits a high methanol permeance (8.10 L m −2 h −1 bar −1 ) and a low molecular weight cut-off (MWCO) of 300 g mol −1 . In addition, the prepared TFC-P[n]a membranes exhibit molecule sieving function and could discriminate molecules with similar molecular weights but different shapes. Our work provides an insight of material design for the preparation of next-generation high-performance organic solvent nanofiltration membranes.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
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CHEMISTRY OF MATERIALS
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2022
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IF 10.508
Yu-Xuan Xiao,Jie Ying,Jiang-Bo Chen,Yuan Dong,Xiong Yang,Ge Tian,Jinsong Wu,Christoph Janiak,Kenneth I. Ozoemena,Xiao-Yu Yang
The heavy d-π effect is an important theoretical model for strong Pt–C interaction, and its enhancement is critical to the high-performance design of Pt/C electrocatalysts. Common chemical N-doping to the carbon support can provide possibilities for enhanced electrocatalysis but most often leads to random interaction with Pt nanoparticles (Pt-NPs) and uncontrollable tuning of the heavy d-π effect. Directional confinement of Pt-NPs within N-doped carbon to directly enhance the heavy d-π effect is therefore mostly preferred but rarely reported. Herein, confined ultrafine Pt-NPs in N-doped porous carbon fibers (Pt@NDPCF) were obtained by a combination method involving electrospinning, carbonization, and directional replacement. Such a synthetic strategy leads to highly dispersed, ultrafine Pt-NPs in hierarchically porous carbon fibers and a strong directional interaction of Pt with pyridinic N, which significantly enhances the heavy d-π effect, greatly facilitating electron transfer and optimizing Pt 5d orbitals. Based on these advances, Pt@NDPCF exhibited outstanding activity and superior durability in the hydrogen evolution reaction (HER), with 24 mV lower overpotential at 10 mA cm–2 and a much smaller activity loss after 10,000 cycles of durability tests in comparison with a commercial Pt/C catalyst. This work sheds new lights on the design of high-performance Pt-based nanomaterials toward HER or other practical applications.
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Catalysts
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2022
·Vol. 12
·期 3
·304
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IF 4.501
Xinxing Gao,Qianqian Pei,Nianqing Zhu,Yi Mou,Jilei Liang,Xin Zhang,Shoushuai Feng
(S)-N-Boc-3-hydroxypiperidine is an important intermediate of the anticancer drug ibrutinib and is mainly synthesized by the asymmetric reduction catalyzed by ketoreductase coupled with glucose dehydrogenase at present. In this study, the coexpression recombinant strainsE. coli/pET28-K-rbs-G with single promoter andE. coli/pETDuet-K-G with double promoters were first constructed for the coexpression of ketoreductase and glucose dehydrogenase in the same cell. Then, the catalytic efficiency ofE. coli/pET28-K-rbs-G for synthesizing (S)-N-Boc-3-hydroxypiperidine was found to be higher than that ofE. coli/pETDuet-K-G due to the more balanced activity ratio and higher catalytic activity. On this basis, the catalytic conditions ofE. coli/pET28-K-rbs-G were further optimized, and finally both the conversion of the reaction and the optical purity of the product were higher than 99%. In the end, the cell-free extract was proved to be a better catalyst than the whole cell with the improved catalytic efficiency of different recombinant strains. This study developed a better coexpression strategy for ketoreductase and glucose dehydrogenase by investigating the effect of activity ratios and forms of the biocatalysts on the catalytic efficiency deeply, which provided a research basis for the efficient synthesis of chiral compounds.Keywords:(S)-N-Boc-3-hydroxypiperidine;coexpression strategy;activity ratio;ketoreductase;glucose dehydrogenase
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Junxian Hu,Yangyang Xie,Jingqiang Zheng,Liuyun Zhang,Hongzhong Li,Yanqing Lai,Zhian Zhang
Metal phosphates are attracting great attention as anode materials for alkali-ion batteries due to their chemical stability, low working voltage, and high theoretical capacity. However, there are few reports on the application of metal phosphate as potassium-ion batteries (PIBs) anode material, and the potassium storage mechanism remains mysterious. Herein, a core–shell chromium phosphate@N-doped carbon (denoted as CrPO 4 @NC) composite is newly synthesized and demonstrated as conversion-type anode material for PIBs. The N-doped carbon coating layer effectively relieves the mechanical strain and improves electrical conductivity during repetitive cycling. The formed P–C bonding between CrPO 4 core and nitrogen-doped carbon shell can help to maintain structural integrity and accelerate charge transfer. As a consequence, the CrPO 4 @NC composite exhibits a decent capacity (304.6 mAh g −1 at 50 mA g −1 ), good rate capability (135.1 mAh g −1 at 500 mA g −1 ), and superior stability (133.2 mAh g −1 at 200 mA g −1 after 100 cycles). Particularly noteworthy, we also provide experimental evidence that a conversion reaction occurs at CrPO 4 @NC electrode with metallic Cr and K 3 PO 4 formed during the potassiation process. This work illustrates that CrPO 4 may be a kind of anode material for applications in energy storage systems.
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AICHE JOURNAL
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2022
·Vol. 68
·期 7
·e17677
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IF 4.167
Shen Hu,Jiaxuan Chen,Qunfeng Zhang,Junru Liu,Jinlin Meng,Guanghua Ye,Xinggui Zhou,Weikang Yuan
Surface barriers persist in the molecular transport across external crystal surface of zeolites, which brings strong influences on zeolite catalysis. This study probes the role of crystal-size–dependent surface barriers in zeolite catalysis, with n -pentane isomerization catalyzed by Pt/ZSM-5 as a model reaction system. Chemical liquid deposition of SiO 2 is performed to reduce surface barriers on ZSM-5 crystals with different sizes. After SiO 2 deposition, surface barriers on both small (266 nm) and large (1304 nm) crystals are significantly reduced, while the improvement in catalytic activity for the large crystals (76.1%–129.1%) is much higher than that for the small ones (−17.4% to 16.7%). For the large ZSM-5 crystals, diffusion limitation is stronger, and thus the effect of surface barriers on catalytic activity is more important. This study reveals the unique role of crystal-size–dependent surface barriers in zeolite catalysis, and understanding this is important for the optimal design of zeolite catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Asim Arshad,Sining Yun,Jing Shi,Menglong Sun,Nosheen Zafar,Anders Hagfeldt
Defect engineering in heterostructured carbon-based electrode materials has evolved as an emerging strategy to boost the electrocatalytic activity. Herein, a facile single-step route is reported to synthesize novel N-coordinated bimetal doped graphitic carbon (Mn/Co-NGC). The formation of M(Mn, Co)-N-C in the catalyst (Mn/Co-NGC) significantly accelerated the triiodide reduction reaction (IRR) and hydrogen evolution reaction (HER). The electrocatalyst provided the synergistic effect of bimetal (Mn, Co)-N active-sites within graphitic-carbon framework, which promoted the conductivity and efficient charge transfer via multiple channels to enhance the IRR and HER. Therefore, as IRR electrocatalyst, Mn/Co-NGC equipped solar-cell attained a superior efficiency of 8.05% compared to Pt (6.82%). The electrocatalyst also exhibited an impressive potential towards HER, providing a low overpoential of 116 mV at 10 mA cm −2 and Tafel slope of 58 mV dec -1 . Moreover, Mn/Co-NGC based solar-cell demonstrated superior stability with 99% efficiency retention (7.96% / 8.05%) after 50 redox-cycles for IRR, and a negligible change in overpotential after 1000 CV cycles. The intrinsic catalytic mechanism of electrocatalysts is studied by insighting their electronic structures, work functions, bonding, and ion-adsorption behaviors, using first-principle DFT-calculations. The current study leads towards designing highly efficient and cost-effective multifunctional electrocatalysts for advanced energy conversion technologies.
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Processes
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2022
·Vol. 10
·期 2
·239
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IF 3.352
Chenghao Li,Lei Ni,Qiang Chen,Juncheng Jiang,Kuibin Zhou
Reaction thermal runaway, caused by excessive temperatures of the reaction system, threatens the safety of operators. Latent heat storage by phase change materials (PCMs) has the advantages of high energy storage density and stable temperature during the energy storage process, which was widely applied in many fields and provides a new idea for the temperature control of thermal runaway reactions. In this study, microencapsulated phase change materials (microPCMs) with a melamine-formaldehybe (MF) resin shell was fabricated by in situ polymerization. The characterization of the micro morphology, chemical bonds, crystal structure, thermal properties, and thermal stability of microPCMs showed that the prepared microPCMs had integrated spherical morphologies and smooth surfaces, with an encapsulation ratio of approximately 70% and good thermal stability. Furthermore, taking the esterification of propionic anhydride (PA) and 2-butanol (2B) as examples,n-octadecane@MF resin microPCMs was used to control the reaction temperature under various operation conditions in semi-batch reactors. The experimental results showed that the mechanism of then-octadecane@MF resin microPCMs on the control of reaction temperature in semi-batch reactors was the combination of both physical and chemical interactions. The applications of microPCMs for the control of reaction temperature hold great potential for use in industrial processes.Keywords:microencapsulated phase change materials;in situ polymerization;reaction inhibitor;temperature control;esterification reaction
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JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Yue Zhao,Huilian Hao,Tianliang Song,Xu Wang,Changwang Li,Wenyao Li
By combining the large power density of supercapacitors with the high energy density of ion batteries , a novel zinc-ion hybrid supercapacitor (ZHSC) is proposed and considered a promising candidate. But there are still challenges in the selection and application of reliable cathode materials . Herein, we used a mature and safe one-step hydrothermal method to synthesize N/P co-doped graphene (NPG), which exhibited a unique three-dimensional structure and a large specific surface area, showing great advantages as cathode to assemble Zn//NPG ZHSC with zinc foil. In the 1 M ZnSO 4 solution, the ZHSC shows superior electrochemical performance, which presents an excellent specific capacitance of 210.2 F g −1 under a wide working voltage of 1.8 V, and it achieves both a maximum energy density of 94.6 Wh kg −1 and a large power density of 4500 W kg −1 . More importantly, the capacitance retention rate remains 82% and a coulomb efficiency of ∼100% is achieved after 15,000 cycles. Overall, the results of this study highlight the efficient synthesis and excellent performance of NPG cathode materials, and also promote the rapid development and great application of high-performance Zn-ion hybrid capacitors.
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Analytical Methods
·
2023
·Vol. 15
·期 27
·3318-3324
·
IF 3.1
Hongyu Chen,Mingshuo Liu,Jianing Wang,Yunfei Wang,Yajuan Wang,Wenyan Liu
Due to their excellent optical and electrical properties, all-inorganic metal halide perovskite CsPbBr3 quantum dots (QDs) have become one of the most promising materials in the field of optoelectronics during recent years. However, the stability of CsPbBr3 QDs limits their practical application and further development to a certain extent. In order to improve their stability, CsPbBr3 QDs were modified with 2-n-octyl-1-dodecanol for the first time in this paper. The 2-n-octyl-1-dodecanol-modified CsPbBr3 QDs were prepared by the ligand-assisted reprecipitation (LARP) method at room temperature in an air environment. Then the stability of the samples was tested at different temperatures and humidity. When the humidity was 80%, the photoluminescence (PL) intensity of both unmodified and modified CsPbBr3 QDs increased to different degrees because the appropriate amount of water changed the crystallization environment. The PL intensity of the modified QDs increased, and the peak positions were basically not shifted, proving that they did not agglomerate. Thermal stability test results showed that the PL intensity of the 2-n-octyl-1-dodecanol-modified QDs could still maintain 65% of the original intensity at 90 °C, which is 4.6 times that of the unmodified CsPbBr3 QDs. Experimental results show that the stability of CsPbBr3 QDs is significantly improved after 2-n-octyl-1-dodecanol modification, which demonstrates the excellent surface passivation of CsPbBr3 QDs by 2-n-octyl-1-dodecanol.
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