Herein, the adsorption performance of sodium montmorillonite (Na-MMT) for amantadine hydrochloride (AMH) was optimized through heat treatment. The removal rate of hydrochloride amantadine by Na-MMT(500) can reach 89.94% under the optimum adsorption conditions of a heat-treatment temperature of 500 degrees C with an initial concentration of AMH of 200 mg L-1. The excellent performance may be plausibly attributed to a synergistic mechanism involving ion exchange, surface hydroxyl complexation, and electrostatic interactions, which are facilitated by thermal-treatment-induced structural reorganization and an increase in the specific surface area.
Herein, a facile strategy for the preparation of PdAgCu ternary nanotubes (NTs) is introduced by using Cu nanowires (NWs) as sacrificial templates along with an acid-leaching treatment. Since the phase separation between Ag and Cu, the obtained PdAgCu NTs is made up of various nanosphases including pure Ag, Cu, bimetallic PdCu and PdAg nanoalloys, instead of PdAgCu trimetallic nanoalloys. By adjusting the types of solvents during synthesis, the surface morphology of PdAgCu NTs can be tuned from smooth (S-PdAgCu NTs) to rough (R-PdAgCu NTs). Both S-PdAgCu NTs and R-PdAgCu NTs exhibit excellent electrocatalytic performances for formic acid oxidation reaction (FAOR). Remarkably, the mass activity of S-PdAgCu NTs for FAOR can reach up to 4307 mA mgPd-1 at peak potential, which is 8.5 times higher than that of commercial Pd (506 mA mgPd impressively enhanced activity should be ascribed to the synergistic effect of Pd with Cu or Ag and the multiphase interface engineering, which is resulting from the tight position relationships among different monometallic or bimetallic alloy nanophases.
Catalytic ozonation process has the advantages of simple operation,high oxidation efficiency and low sec-ondary pollution in the advanced treatment of phenol containing organic wastewater.However,its large-scale appli-cation depends on the development of heterogeneous catalysts with high activity and stability.Herein,the mecha-nism of hetergeneous catalytic ozone oxidation reaction in catalytic ozonation technology was introduced.The re-search status of heterogeneous catalysts for catalytic ozonation of phenolic compounds was reviewed from two as-pects of non-supported and supported catalysts,and the characteristics and limitations of non-supported catalysts,single active component supported catalysts and multi-component supported catalysts were mainly analyzed.Multi-component supported catalyst is the main research object since its advantages on improving ozone utilization rate,re-ducing ozone emission and great potential of performance optimization.To develop highly efficient catalysts,the opti-mization strategy on composition,size and defect site of catalyst was proposed from the perspective of geometric structure and electronic structure.Finally,the research progress of heterogeneous catalytic ozonation catalysts for re-moval of phenolic compounds was summarized and prospected in order to provide reference for the development of efficient catalysts for catalytic ozonation technology.
Atomically dispersed metal catalysts including single-atom catalysts (SACs) and dual-atom catalysts (DACs) are needed to be developed for the sluggish oxygen evolution reaction (OER) in the field of energy conversion and utilization. Modification of the coordinating environment of the active sites and changing the OER are effective strategies to improve the catalytic activity of SACs and DACs. In this work, in order to improve the OER activity, the coordination environment of the active sites in SACs and DACs is changed by doping B/O/P atoms and the P atom, respectively. The catalytic activity and stability of SACs Mn-N-C, DACs FeMn-N-6-C, and DACs FeMn-N-7-C in various coordination environments are studied by density functional theory. Calculation results suggest that the doping of heteroatoms in SACs Mn-N-C and DACs FeMn-N-7-C can effectively enhance the catalytic activity. The unique double active sites of DACs can avoid the formation of OOH* that often occurs as the reaction rate-determining step in the traditional reaction pathway to change the reaction pathway and improve its OER catalytic activity. Moreover, DACs FeMn-N-6-C with ultralow theoretical overpotential (0.14 V) are considered to be one of the compounds with excellent OER catalytic activity. The reaction pathway as well as the coordination regulation in the atomically dispersed metal catalysts can help to understand and design new OER electrocatalysts. Our study also provides new insights into the emerging new atomically dispersed metal catalysts for efficient energy electrocatalysis.
The construction of highly efficient and low-cost catalysts is crucial for the reduction reaction of 4-nitrophenol (4-NP). Herein, we provide a simple processing method, including vacuum storage, natural oxidation, and heating oxidation, that effectively regulates the surface oxidation state of copper nanowires and produces copper nanowires with different oxidation states (such as Cu, Cu2O, and CuO). Research has found that CuNW-N (Cu nanowires for vacuum storage) catalysts with a surface composition of 67.9% Cu0, 20.6% Cu+, and 11.5% Cu2+ exhibit the best catalytic performance for the reduction of 4-nitrophenol (4-NP) and their reaction rate constant reaches 0.791 min-1. This work provides a feasible catalyst preparation strategy for the efficient catalytic reduction of 4-NP. Graphical Abstract Herein, we obtain copper nanowires with different oxidation states (such as Cu, Cu2O, and CuO). Research has found that CuNW-N catalysts with a surface composition of 67.9% Cu0, 20.6% Cu+, and 11.5% Cu2+ exhibit the best catalytic performance for the reduction of 4-nitrophenol (4-NP) and their reaction rate constant reaches 0.791 min-1.
Atomically dispersed catalysts (ADCs), including single atoms and sub-nanoclusters, simultaneously, are considered as the most promising candidate to boost the reaction kinetics of hydrogen evolution reaction (HER). However, the correlation between the coordination environment of single atoms and catalytic activity has not been clearly discussed in ADCs system. Herein, Pt ADCs with the different coordination structures were fabricated by a facile sulfurate route coupling deposition strategy. Importantly, Pt ADCs, including Pt-O1Ni1 single atoms and Pt sub-nanoclusters (Pt1+n/Ni3S2), show good basic HER activity, which just need 17 mV at 10 mA cm(-2). Meanwhile, the turnover frequency for Pt1+n/Ni3S2 is 0.49 H-2 s(-1) under the overpotential of 100 mV, which is 8.6 times higher than Pt/C. Besides, the assembled RuO2 ||Pt1+n/Ni3S2 system could get 100 mA cm(-2) current density under 1.7 V cell voltage in alkaline water electrolyzer. Notably, in-situ Raman and attenuated total reflection-surface enhanced infrared absorption spectroscopy reveal that Pt-O1Ni1 coordination is conducive to promoting the fracture of H-O-H bond, realizing the rapid transform of Pt-H* intermediates. Further, density functional theory calculations confirm Pt single atoms with Pt-O1Ni1 coordination environment in Pt1+n/Ni3S2 serves as the main role for HER because Pt-O1Ni1 are more likely to accelerate the production of Pt-H* at the Pt sites, extremely achieving the rapid HER progress. This work discloses the structure-activity relationship in ADCs system, which is essential for the development of highly active electrocatalysts.
Herein, Al2O3 supported ultra-small Mn-CeOx nanoparticles (Mn-CeOx/Al2O3) are prepared by a facile impregnation method for removal of phenolic compounds via catalytic ozonation. Mn and Ce species are in the form of polyvalent oxide nanoparticles with an average size of 0.9 nm. The removal efficiency of total organic carbon for phenol-containing model wastewater by Mn-CeOx/Al2O3 shows a volcano relationship by changing the mass ratio of Mn and Ce, and reaches up to the peak value when the mass ratio is 5:5. The cycle stability tests suggest the removal efficiency of Mn-CeOx/Al2O3 could maintain at 90.16 % after 5 circles. The enhanced performance should be attributed to the optimized magnetism and accelerated charge transfer by composition regulation. The magnetic strength changing affects the adsorption mode of O3, while the redox cycle of Mn(IV)/ Mn(III) and Ce(IV)/Ce(III) could enhance the activation of O3 to produce more & sdot;OH and 1O2 for the organic molecules mineralization.
Regulating catalyst composition is one of the efficient approaches to boost intrinsic activity of electrocat-alysts for water splitting. Herein, four different hollow porous platinum-copper (PtCu) nanotubes (NTs) with controllable compositions were precisely fabricated by a facile wet-chemistry method. Importantly, Pt5Cu2 NTs display the best hydrogen evolution reaction (HER) performance in all pH con-ditions compared to other samples, which just require overpotentials of 34 +/- 2, 32 +/- 2, and 284 +/- 2 mV at 10 mA cm(-2) in basic, acidic, and neutral solutions, respectively. Moreover, Pt5Cu2 NTs also exhibit out-standing stability and corrosion resistance in all pH ranges. Then, mechanism analysis reveals that the electronic structure of Pt sites is regulated by changing the ratio of Pt and Cu, which directly optimizes the binding energy of reaction intermediates and promotes electron transfer during the HER process. In addition, a porous nanotube structure with countless nanoparticles on the surface provides a large num-ber of active sites, enhancing the adsorption/desorption of reactants. This work emphasizes the impor-tance of catalyst composition and provides a highly active potential HER catalyst for practical hydrogen production. (C) 2022 Elsevier Inc. All rights reserved.
Developing low-cost and high-performance adsorbents is of great significance for the treatment of wastewater containing heavy metal ions. Herein, dodecyl dimethyl betaine modified Na-based montmorillonite (BS-MMT) is successfully prepared by a facile wet method for enhanced lead ion (Pb2+) adsorption. The interlamellar spacing of Na-MMT is effectively regulated ranges from 1.25 to 1.79 nm by changing the ratio of BS-12 content from 5% to 150% (vs. MMT). The Pb2+ capacity adsorption of BS-MMT could reach up to 255.36 mg/g when the usage of BS-12 is 15%. Pb2+ adsorption process on BS-MMT follows the Langmuir model and is endothermic. Mechanism analysis suggests that the main Pb2+ adsorption pathways on BS-MMT include ion exchange, functional group complexation, electrostatic attraction and precipitation by CO3 2 . Moreover, the modification of BS-12 could not only brings carboxyl and amine functional groups to trap of Pb2+ on the surface and interlayer of MMT, but also optimize the layer spacing of MMT since its long carbon chain. This work provides a feasible strategy to optimize the adsorption capacity of organic modified MMT for heavy metals.
Innovene S高密度聚乙烯(HDPE)装置在使用进口MT钛催化剂期间,装置存在反应器轴流泵功率快速增加、生产周期短以及无法提高生产负荷等问题.通过试用国内外钛系催化剂,研究国内外钛系催化剂在高密度聚乙烯双峰产品中的应用,比较国内外钛系催化剂的活性和对反应器操作条件、产品性能的影响.试验结果表明,BCL 和 SEL 国产催化剂的活性比进口催化剂高约60%~80%,聚合物粉料粒径分布窄,流动性更好,生产的树脂力学性能与进口催化剂相当,有利于装置更高的负荷稳定生产;使用国产催化剂可以延长袋式过滤器使用周期,轴流泵功率稳定,提高经济效益,很好地解决了进口MT钛系催化剂目前存在的问题.
Fabricating highly efficient and low-cost absorbents to remove organic contaminants in industrial effluents is urgent yet of great importance. Herein, a facile one-pot hydrothermal approach was developed to successfully construct magnesium silicate and bentonite composite (MS-Bt) with uniform multilayer porous structure by using Bt as structural promoter. The specific surface area of MS-Bt can reach up to 392 m2 center dot g-1 along with an average pore diameter of 2.29 nm and a pore volume of 0.22 cm3 center dot g-1. MS-Bt composite exhibits a maximal adsorption capacity of 253.92 mg center dot g-1 for methylene blue (MB) in model wastewater treatment. Adsorption behavior fitted well with Langmuir isotherm and pseudo-second-order kinetics adsorption equations. The adsorption pathways of MB on MS-Bt mainly include chemical precipitation by Mg-OH, electrostatic attraction and surface hydroxyl functional group capture. This work is anticipated to give a new insight into constructing organic contaminants adsorbent by using clay mineral material as an auxiliary agent.
一维铜(Cu)基合金纳米催化剂具有高活性、高化学稳定性及良好的导电性等优点,在催化材料领域得到广泛研究.本文介绍了一维Cu基合金纳米催化剂的制备方法,重点综述了用于电解水制氢的一维合金Cu基纳米催化剂的研究进展与性能特点,从不同角度阐述了催化剂性能优化策略,包括催化剂形貌与结构、活性位电子与几何结构等,最后对一维Cu基合金纳米催化剂在电解水中的应用前景进行了展望.
A zeolitic imidazole framework-8/montmorillonite (ZIF-8/MMT) composite was synthesized by a simple method through in-situ growth of ZIF-8 on MMT for efficient Pb2+ capture from water. The adsorption process of Pb2+ by ZIF-8/MMT composite followed the Langmuir model and the maximum adsorption could reach up to 336.89 mg/ g, which was much better than that of the monocomponent of ZIF-8 (117.78 mg/g) or MMT (85.20 mg/g). Kinetics result suggested that Pb2+ adsorption by ZIF-8/MMT was a pseudo-second-order dynamic process, indicating a chemisorption process dominates. Ion exchange, electrostatic attraction and hydroxyl complexation were main pathways for Pb2+ removal by ZIF-8/MMT composite. The enhanced performance of ZIF-8/MMT composite should be attributed to following points. Firstly, the lamellar structure of MMT was in favor of ZIF-8 nanoparticles grow and disperse uniformly on the surface, thus avoiding the aggregation. Secondly, the pos-itive charge on ZIF-8 was neutralized by the negative charge on the surface of MMT, and thus the adsorption capacity of ZIF-8 for Pb2+ is effectively released. Thirdly, the combination of MMT and ZIF-8 optimized the pore structure, which was favorable for Pb2+ adsorption and diffusion. Therefore, the synthesized ZIF-8/MMT com-posites is a prospective candidate for Pb2+ removal from wastewater.
Constructing efficient bifunctional electrocatalysts for both cathode and anode is of great importance for obtaining green hydrogen by water splitting. Herein, sulfuration of hierarchical Mn-doped NiCo LDH heterostructures (Mn-NiCoS2/NF) is constructed as a bifunctional electrocatalyst for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) via a facile hydrothermal-annealing strategy. Mn-NiCoS2/NF shows an overpotential of 310 mV at 50 mA cm-2 for OER and 100 mV at 10 mA cm-2 for HER in 1.0 M KOH. Moreover, only 1.496 V@10 mA cm-2 is required for overall water splitting by using Mn-NiCoS2/NF as catalyst dual electrodes in a two-electrode system. The excellent performance of Mn-NiCoS2/NF should be attributed to the ameliorative energy barriers of adsorption/desorption for HO-/H2O through the modification of electronic structure of NiCo basal plane by Mn-doping and the acceleration of water dissociation steps via rich delocalized electron inside sulfur vacancies. The construction of hierarchical Mn-NiCoS2/ NF heterostructures provides new prospects and visions into developing efficientadvanced electrocatalysts for overall water splitting. & COPY; 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Developing bifunctional electrocatalysts with lowcontent noble metals and high activity and stability is crucial for water splitting. Herein, we reported a novel Ru doped FeP4/Fe2PO5 heterogeneous interface catalyst (Ru@FeP4/Fe2PO5) for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) by heat treatment coupling electrodeposition strategy. Experiments disclosed that Ru@FeP4/Fe2PO5 proclaimed excellent catalytic activity for the OER (249 mV@100 mA cm(-2)) and HER (49 mV@ 10 mA cm(-2)) in a 1 M KOH environment. More importantly, the mass activity and turnover frequency of Ru@FeP4/Fe2PO5 were 117 and 108 times higher than that of commercial RuO2 at an overpotential of 300 mV during the OER, respectively. In addition, the assembled Ru@FeP4/Fe2PO5 || Ru@FeP4/Fe2PO5 system could retain superior durability in a two-electrode system for 134 h at 300 mA cm(-2). Further mechanism studies revealed that Ru atoms in Ru@FeP4/Fe2PO5 act in a key role for the excellent activity during water splitting because the electronic structure of Ru sites could be optimized by the interaction between Ru and Fe atoms at the interface to strengthen the adsorption of reaction intermediates. Besides, the introduction of Ru atoms could also enhance the charge transfer, which effectually accelerates the reaction kinetics. The strategy of anchoring Ru atom on novel heterostructure provides a promising path to boost the overall activity of electrocatalysts for water splitting.
在Innovene S双环管低压淤浆工艺装置上,采用国产NTR型催化剂生产了高密度聚乙烯,利用粒度分析、熔融指数测试、GPC、力学性能测试等考察了催化剂的性能、反应器工况以及树脂的力学性能和加工性能,并与进口催化剂进行了对比.试验结果表明,试用NTR型催化剂期间,装置运行平稳,满足长周期运行要求.NTR型催化剂的粒径大,比表面积高,活性高于进口催化剂,可以降低反应器中粉料溶解结垢的风险,可用于开发更高熔融指数的产品.生产的树脂粉料细粉含量较低,高分子量颗粒占比相对较多.与进口催化剂生产的树脂相比,拉伸性能、刚性及黄色指数接近,气味及外观颜色正常,表观剪切黏度略高、熔体强度略低,分子量分布接近,耐环境应力开裂性能较好.树脂加工性能良好,吹塑成品在中空成型加工测试中均能达到优级品质量标准.
以河南南部天然钙基膨润土为原料,通过钠化改性得到了钠基膨润土.通过调控吸附剂用量、亚甲基蓝(MB)浓度、吸附时间、溶液pH值和温度,分析对比了天然钙基膨润土(PRT-1)、钙基提纯膨润土(PRT-1T)和钠基膨润土(PRT-1Na)对MB的去除效率.同时,对PRT-1T和PRT-1Na对MB的吸附动力学和吸附机制进行了研究.结果表明,由于PRT-1Na有更大的比表面积、更高的阳离子交换容量和更丰富的羟基结构,表现出对MB更好的吸附效果.在同等吸附条件下,PRT-1Na的吸附效果是PRT-1的4倍,PRT-1T是PRT-1的2倍.在20℃,pH为6,PRT-1Na用量为1.0 g,吸附时间为2 h,MB为500 mL,且初始浓度为500 mg·L-1时,MB去除率高达99.89%.另外,PRT-1Na对MB染料废水的吸附既存在物理吸附也有化学吸附,Elovich模型对PRT-1T和PRT-1Na吸附MB染料废水的过程拟合度均高,但伪一级动力学模型对PRT-1Na拟合效果最好.
Developing efficient and low-cost adsorbent for removing heavy metal ions from aqueous solution is of great significance for environmental protection. Herein, low quality natural bentonite was purified and sodium-modified to adsorb Pb2+ from the aqueous phase. The effects of initial pH value of the solution, type and amount of the adsorbent, contact time and initial Pb2+ concentration on the adsorption performance of sodium bentonite were systematically studied. The adsorption efficiency of sodium bentonite was significantly better than that of purified bentonite and natural bentonite toward Pb2+. Under the optimum adsorption conditions of pH = 5, adsorbent dosage of 0.2 g, initial Pb2+ concentration of 400 mg/L, and adsorption time of 120 min, sodium bentonite can remove more than 99.94% of Pb2+. Adsorption behavior fitted well with Freundlich isotherm and pseudo-second-order kinetics adsorption equations. Adsorption process was endothermic and feasible. The adsorption pathways of Pb2+ on sodium bentonite are mainly including ion exchange, surface hydroxyl functional group capture, electrostatic attraction and chemical precipitation by CO32- in the pore channel to form PbCO3. This research is anticipated to give technical support for prompting the wider application of bentonite as an adsorbent material.
Constructing highly efficient and low cost electrocatalysts for oxygen evolution reaction (OER) is pivotal to various energy storage and conversion devices. In this work, five different rare earth (RE) metals doped (La, Ce, Pr, Nd, Er) Ag-nanoparticles-decorated alpha-Co(OH)(2) nanostructured electrocatalysts, which are grown on nickel foam (NF), are successfully prepared by a facile one-step hydrothermal approach. It is found that La-doped 2D ultrathin (similar to 2.0 nm) CoAg nanosheets arrays (denoted as La-CoAg/NF) can demonstrate the highest electrochemical activity towards OER in 1 M KOH solution among these RE-doped electrocatalysts. It delivers the lowest overpotential at 10 mA cm(-2) (233 mV), the smallest Tafel slope (44.3 mV dec(-1)) and extraordinary stability for 35 h with no significant change during harsh OER process. The reasons for the enhanced performance may come from unique ultrathin 2D nanostructure and La-induced strong electronic interaction among Co, Ag, and La atoms. This work provides an essential insight to the development of RE-metal doped electrocatalysts for energy conversion. (C) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Herein, α-Al2O3 supported Ag particles with controllable size distribution are prepared successfully by tuning of the calcination conditions through an impregnation method. The size of Ag particles could be adjusted by changing the calcination time and temperature. The catalyst samples were analyzed by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and other characterization methods under different calcination conditions, and the performance differences of their catalytic reduction of p-nitrophenol (4-NP) were investigated by UV-Vis spectroscopy. The results show that the Ag particles with increased particle size can be obtained on the surface of α-Al2O3 support by increasing the calcination time or calcination temperature. The catalytic performance of the samples obtained by increasing the calcination time decreased, while the catalytic performance of the samples obtained by increasing the calcination temperature increased. This may be due to the interaction between Ag particles and the support, which changes the valence state of Ag species. Also the particle size effect acts on the catalyst and affects its catalytic performance together with the change of valence.