Nickel(II) ion-intercalated MXene membranes for enhanced H2/CO2 separation

Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H₂. Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni²⁺ were assembled to form an MSM supported on Al₂O₃ hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H₂/CO₂ mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 10⁻⁸ mol·m⁻²·s⁻¹·Pa⁻¹. Compared with the original Ti₃C₂T_x/Al₂O₃ hollow fiber membranes, the permeation of hydrogen through the Ni²⁺-Ti₃C₂T_x/Al₂O₃ membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni²⁺. The interlayer spacing of MSMs was tuned by Ni²⁺. During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni²⁺ tailored Ti₃C₂T_x/Al₂O₃ hollow fiber membranes can inspire promising industrial applications.     

Synthesis of Chl@Ti3C2 composites as an anode material for lithium storage

Two-dimensional (2D) titanium carbide MXene Ti₃C₂ has attracted significant research interest in energy storage applications. In this study, we prepared Chl@Ti₃C₂ composites by simply mixing a chlorophyll derivative (e.g., zinc methyl 3-devinyl-3-hydroxymethyl- pyropheophorbide a (Chl)) and Ti₃C₂ in tetrahydrofuran, where the Chl molecules were aggregated among the multi-layered Ti₃C₂ MXene or on its surface, increasing the interlayer space of Ti₃C₂. The as-prepared Chl@Ti₃C₂ was employed as the anode material in the lithium-ion battery (LIB) with lithium metal as the cathode. The resulting LIB exhibited a higher reversible capacity and longer cycle performance than those of LIB based on pure Ti₃C₂, and its specific discharge capacity continuously increased along with the increasing number of cycles, which can be attributed to the gradual activation of Chl@Ti₃C₂ accompanied by the electrochemical reactions. The discharge capacity of 1 wt-% Chl@Ti₃C₂ was recorded to be 325 mA·h·g^–1 at the current density of 50 mA·g^–1 with a Coulombic efficiency of 56% and a reversible discharge capacity of 173 mA·h·g^–1 at the current density of 500 mA·g^–1 after 800 cycles. This work provides a novel strategy for improving the energy storage performance of 2D MXene materials by expanding the layer distance with organic dye aggregates.     

The prior rules of designing Ti3C2Tx MXene-based gas sensors

Working temperature, sensitivity, and selectivity are some of the characteristics of the applied gas sensors. How to design and fabricate an ideal gas sensor working at room temperature is still challenging and attracting lots of interest. Two-dimensional (2D) materials with ultra-thin structure have been demonstrated as a family of ideal candidates to achieve this goal. Among them, Ti₃C₂T_x MXene, a kind of layered sheet synthesized by selectively etching MAX phases materials, shows remarkable potential to be the sensitive materials solely or in a composite. However, their designing rules are still lacking critical thinking from the viewpoint of the intrinsic property of Ti₃C₂T_x MXene based materials. In this article, two critical features, i.e., the thickness of the sensitive materials, and the scope of the analytes, are elaborated towards Ti₃C₂T_x MXene based gas sensors after characterizing the performance of sensing reducing gases (NH₃ and CO) and oxidizing gas (NO₂). First, the thinner the Ti₃C₂T_x MXene sensitive layer, the better the sensitivity. Second, the Ti₃C₂T_x MXene based gas sensor is not suitable for strong and moderate oxidation gas due to its ease of oxidation. These two rules are demonstrated, and could be considered with priority both in the future researches and practical applications.     

一步法合成二维Ti3C2及其电化学性能研究

二维过渡金属碳/氮化物（MXene）是一种新型二维材料,可通过从MAX相前体中选择性刻蚀 A 原子层获得。在传统制备MXene的方法中,常用的刻蚀剂是氢氟酸。然而高浓度氢氟酸的使用,不可避免会带来安全问题,甚至破坏MXene的晶体结构,从而限制本征物理化学性能。从典型的碳化物前体Ti₃AlC₂出发,使用 NH₄BF₄作为刻蚀剂,有效降低体系中酸的使用量;在反应过程中,刻蚀 A 层的同时,\mathrm{N}{\mathrm{H}}_{\mathrm{4}}^{+}进入堆垛层间,扩大层间距,弱化层间作用力。因此,仅通过简单手摇就可以实现高效剥离,得到具有完整晶体结构的二维Ti₃C₂。进一步测试了Ti₃C₂的电化学性能,结果显示,所得的Ti₃C₂具有优异的性能（扫描速率为5 mV?s^-1时为503 F?g^-1）和循环稳定性（在5 A?g^-1下循环10⁴次后电容保持率为95.8%）。本文为Ti₃C₂纳米片的合成及应用提供了新的思路。     

Enhanced adsorption of phenol from aqueous solution by carbonized trace ZIF-8-decorated activated carbon pellets

Trace zeolitic imidazolate framework-8(ZIF-8)-decorated activated carbon(AC) pellets were synthesized by a facile wet impregnation technique. After pyrolysis of the above composite material, the obtained carbon had a large surface area and pore volume, with traces of Zn on its surface. Subsequently, the capacity of the ZIF8/AC samples to adsorb and remove phenol from aqueous media was evaluated in both batch and column experimental setups. The equilibrium adsorption capacity reached 155.24 mg·g~(-1), which was 2.3 times greater than that of the pure AC(46.24 mg·g~(-1)). In addition, adsorption kinetics were examined by pseudofirst and pseudosecond order models, and adsorption isotherms were fitted into Langmuir and Freundlich equations. The adsorbent could be easily filtered from the solution and washed with methanol and water, while maintaining an efficiency N 90% after 4 cycles. The above results make it a potentially reusable candidate for water purification.     

Spray-drying assisted layer-structured H2TiO3 ion sieve synthesis and lithium adsorption performance

A spray-drying assisted solid-state method to prepare spherical layer-structured H₂TiO₃ ion sieve (LSTIS) particles is reported herein. The effects of synthesis parameters (calcination temperature, calcination time, and the lithium-titanium molar ratio) on adsorption–desorption performance (the delithiation ratio, titanium dissolution loss, and the adsorption capacity) were investigated. The as-prepared LSTIS exhibited an equilibrium adsorption capacity of 30.08 mg·g^-1 (average of 25.85 mg·g^-1 over 5 cycles) and ultra-low titanium dissolution loss of less than 0.12% (average of 0.086% over 5 cycles). The LSTIS showed excellent selectivity toward Li⁺ in Na⁺, K⁺, Mg²⁺, and Ca²⁺ coexisting saline solutions where its adsorption capacity reached 27.45 mg·g^-1 and the separation factors of Li⁺ over the coexisting cations exceeded 100. The data suggests that the LSTIS is promising to competitively enrich Li⁺ from saline solutions.     

Conversion of Malaysian low-rank coal to mesoporous activated carbon: Structure characterization and adsorption properties

Malaysian Selantik low-rank coal (SC) was used as a precursor to prepare a form of mesoporous activated carbon (SC-AC) with greater surface area (SA) via a microwave induced KOH-activation method. The characteristics of the SC and SC-AC were evaluated by the iodine number, ash content, bulk density, and moisture content. The structure and surface characterization was carried out using pore structure analysis (BET), scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDX), X-ray diffraction (XRD), Fourier Transform Infrared (FTIR), elemental analysis (CHNS), thermogravimetric analysis (TGA), and determination of the point of zero charge (pH_PZC). These results signify a mesoporous structure of SC-AC with an increase of ca. 1160 times (BET SA=1094.3 m²·g^-1) as compared with raw SC without activation (BET SA=1.23 m²·g^-1). The adsorptive properties of the SC-AC with methylene blue (MB) was carried out at variable adsorbent dose (0.2-1.6 g·L^-1), solution pH (2-12), initial MB concentrations (25-400 mg·L^-1), and contact time (0-290 min) using batch mode operation. The kinetic profiles follow pseudo-second order kinetics and the equilibrium uptake of MB conforms to the Langmuir model with a maximum monolayer adsorption capacity of 491.7 mg·g^-1 at 303 K. Thermodynamic functions revealed a spontaneous endothermic adsorption process. The mechanism of adsorption included mainly electrostatic attractions, hydrogen bonding interaction, and π-π stacking interaction. This work shows that Malaysian Selantik low-rank coal is a promising precursor for the production of low-cost and efficient mesoporous activated carbon with substantive surface area.     

Potential-aided recovery of iodide using 2-D nanosheet CuxO coating polymer/graphene/carbon fibers composite

2-D nanosheet Cu_2O doped CuO coating poly m-phenylenediamine and melamine/graphene/carbon fibers composite(Cu_xO/MPM/GFs) was firstly fabricated by compound electrochemical method. Cu_xO/MPM/GFs was successfully used to the recovery of iodide(I~-) from salt water by lower potential-aided sorption and desorption processes. The potential-aided recovery of I~- at CuxO/MPM/GFs was characterized by FE-SEM, XRD, IR, Raman,XPS, UV–vis and electrochemical techniques in detail. The maximal adsorption capacity of 86.82 mg·g~(-1) could be obtained with a pseudo-second-order model at 0.8 V for 210 min in pH 5.0, 0.1 mol·L~(-1) NaCl, and the process accompanied the generation of CuI, CuO and I~(5-). The I-could be quickly desorbed from the electrode with a transfer of CuI to Cu_2O by cycle voltammetry from -1.0 to 0.5 V for 90 cycles in pH 9.0, 0.1 mol·L~(-1) KNO_3.Thus, CuxO/MPM/GFs was renewable in the continuous electrochemical-adsorption–desorption processes.     

A pillared-layer metal-organic framework for efficient separation of C3H8/C2H6/CH4 in natural gas

Metal-organic frameworks (MOFs) have great potentials as adsorbents for natural gas purification. However, the trade-off between selectivity and adsorption capacity remains a challenge. Herein, we report a pillared-layer metal-organic framework Ni(HBTC)(bipy) for efficiently separating the C₃H₈/C₂H₆/CH₄ mixture. The experimental results show that the adsorption capacity of C₃H₈ and C₂H₆ on Ni(HBTC)(bipy) are as high as 6.18 and 5.85 mmol·g^-1, while only 0.93 mmol·g^-1 for CH₄ at 298 K and 100 kPa. Especially, the adsorption capacity of C₃H₈ at 5 kPa can reach an unprecedented 4.52 mmol·g^-1 and for C₂H₆ it is 1.48 mmol·g^-1 at 10 kPa. The ideal adsorbed solution theory predicted C₃H₈/CH₄ selectivity is as high as 1857.0, superior to most of the reported materials. Breakthrough experiment results indicated that material could completely separate the C₃H₈/C₂H₆/CH₄ mixture. Therefore, Ni(HBTC)(bipy) is a promising material for separation of natural gas.     

MXene@CS复合絮凝剂的制备及其对刚果红去除的研究

壳聚糖（CS）因具有大量的羟基和氨基,可为吸附色素污染物提供较多活性位点,但其在酸性条件易于溶解。MXene可为CS提供支撑位点,从而构建新型MXene@CS复合材料。研究构建了新型Ti₃C₂T_X@CS有机无机复合材料,并应用于刚果红的去除研究。通过对Ti₃C₂T_X@CS的微观形貌、晶体结构、表面官能团等进行表征分析,发现Ti₃C₂T_X@CS的复合过程为物理复合。絮凝实验结果表明：在Ti₃C₂T_X@CS投加量为30 mg、溶液pH为9、反应时间为30 min、温度为25~60 ℃条件下,Ti₃C₂T_X@CS对50 mL质量浓度为500 mg/L刚果红（CR）溶液的脱色率达到99%以上。通过实验结果和反应前后Ti₃C₂T_X@CS电位变化推断,Ti₃C₂T_X@CS对刚果红的去除机理主要是电中和作用和吸附架桥作用。     

污泥含炭吸附剂的制备及其吸附模拟烟气中汞蒸汽的应用(英文)

The carbonaceous adsorbent was prepared from mixtures of dewatered sludge and sawdust with enhanced ZnCl2 chemical activation.Characteristics of the adsorbent were studied using scanning electron microscope(SEM) ,Fourier transform infrared spectroscopy(FT-IR) ,and adsorption of nitrogen.The surface analysis showed that the carbonaceous adsorbent had good specific surface and porosity(394 m 2 ·g-1of BET surface,0.12 and 0.10 ml·g-1of microporous and mesoporous volume,respectively) .The oxygen functional groups such as OH,C O and C O were found on the surface by FTIR and XPS(X-ray photoelectron spectroscopy) .The adsorption of elemental mercury(Hg0) on the carbonaceous adsorbent was studied in a fixed bed reactor.The dynamic adsorption capacity of carbonaceous adsorbent increased with influent mercury concentration,from 23.6μg·g-1at 12.58μg·m-3to 87.9μg·g-1at 72.50μg·m-3,and decreased as the adsorption temperature increased,from 246 μg·g-1 at 25°C to 61.3μg·g-1 at 140°C,when dry nitrogen was used as the carrier gas.The carbonaceous adsorbent presented higher dynamic adsorption capacity than activated carbon,which was 81.2μg·g-1and 53.8μg·g-1respectively.The adsorption data were fitted to the Langmuir adsorption model.The physical and chemical adsorption were identified on the adsorbent.     

Synthesis of a novel functional group-bridged magnetized bentonite adsorbent:Characterization,kinetics, isotherm,thermodynamics and regeneration

A novel magnetic adsorbent was synthesized by magnetizing bentonite by APTES-Fe_3O_4 via a functional groupbridged interaction. The characterization of APTES-Fe_3O_4/bentonite was conducted via transmission electron microscope(TEM), X-ray diffraction(XRD), Fourier transform infrared spectrophotometer(FT-IR), thermal gravimetric analysis(TGA), vibrating sample magnetometer(VSM), zeta potential analysis and Brunner–Emmet–Teller(BET). The APTES-Fe_3O_4/bentonite was assessed as adsorbents for methylene blue(MB) with a high adsorption capacity(91.83 mg·g~(-1)). Factors affecting the adsorption of MB(such as p H, equilibrium time, temperature and initial concentration) were investigated. The adsorption process completely reaches equilibrium after 120 min and the maximum sorption is achieved at p H 8.0. The adsorption trend follows the pseudosecond order kinetics model. The adsorption data gives good fits with Langmuir isotherm model. The parameter factor RLfalls between 0 and 1, indicating the adsorption of MB is favorable. The adsorption process is endothermic with positive ΔH~0 values. The positive values of ΔG~0 confirm the affinity of the adsorbent towards MB, and suggest an increased randomness at the solid–liquid interface during the adsorption process. Regeneration of the saturated adsorbent was easily carried out via gamma-irradiation.     

Protein-derived nitrogen and sulfur co-doped carbon for efficient adsorptive removal of heavy metals

A nitrogen and sulfur co-doped carbon has been synthesized employing egg white as a sustainable protein-rich precursor. According to CHNS elemental analysis, N, S and O heteroatoms accounted for mass fractions of 3.66%, 2.28% and 19.29% respectively, and the types of surface functionalities were further characterized by FT-IR and XPS measurements. Although the carbon possessed a smaller surface area (815 m²·g^-1) compared to a commercial activated carbon (1100 m²·g^-1), its adsorption capacity towards Co²⁺ reached 320.3 mg·g^-1, which was over 8 times higher compared to the limited 34.0 mg·g^-1 over the activate carbon. Furthermore, the carbon was found to be an efficient adsorbent towards a series of metal ions including VO²⁺, Cr³⁺, Ni²⁺, Cu²⁺ and Cd²⁺. Combined with its environmental merits, the protein derived carbon may be a promising candidate for heavy metal pollution control.     

g-C3N4的改性策略以及g-C3N4/Ti3C2异质结研究进展

石墨相氮化碳（g-C₃N₄）禁带宽度约为2.7 eV，具有可见光响应能力。由于其良好的热和化学稳定性，且形貌和化学结构可调，在光催化领域应用广泛。但由于其带隙宽，对可见光响应范围窄，且光生载流子的复合率高，导致其光催化效率低，可通过改性来改善。本文综述了对g-C₃N₄形貌调控、掺杂和构建异质结等改性策略，以及g-C₃N₄/Ti₃C₂异质结的作用机理、制备方法和在光催化析氢、有机物降解及合成等领域的应用。     

Research progress on modification strategy of g-C3N4 and g-C3N4/Ti3C2 heterojunction

Graphite phase carbon nitride (g-C₃N₄) is a kind of metal-free semiconductor material with a forbidden band width of about 2.7 eV and has visible light response capability. Attributed to its good thermal and chemical stability, adjustable morphology and chemical structure, it is widely used in the field of photocatalysis. However, due to its low specific surface area and wide band gap, its response range to visible light is narrow and the recombination rate of photogenerated carriers is high, resulting in a low photocatalytic efficiency, which can be effectively improved by modification. The two-dimensional material Ti₃C₂ has a narrower band gap compared with other semiconductor materials, and the heterogeneous junction between Ti₃C₂ and g-C₃N₄ is expected to obtain a wider range of visible light absorption and higher photocatalytic efficiency. This article reviews the modification methods of g-C₃N₄ including morphology control, doping and constructing heterojunctions, as well as the action mechanism, preparation methods and applications of g-C₃N₄/Ti₃C₂ heterojunction in photocatalytic hydrogen evolution, organics degradation and synthesis, etc.     

Multivariate optimization of high removal of lead(Ⅱ) using an efficient synthesized Ni-based metal–organic framework adsorbent

A new metal-organic framework(MOF) with the chemical formula of [Ni_2 F_2(4,4'-Bipy)_2(H_2 O)_2](VO_3)_2·8 H_2 O was introduced to adsorb Pb(Ⅱ) with the highest capacity.The sorbent was characterized by thermogravimetric analysis(TGA),infrared spectroscopy(FT-IR),field-emission scanning electron microscopy(FESEM),energy-dispersive Xray(EDX),and elemental analysis.The optimum conditions were obtained by a face-centered central composite design(FCCD) as follows:adsorbent dosage(m)=1.2 mg, initial concentration of Pb(Ⅱ)(C)=390 mg·L~(-1),and pH=5.According to the Langmuir model(R~2=0.9999),the maximum monolayer uptake capacity of lead(Ⅱ) is 2400.7 mg·g~(-1),which is the highe st observed amount for lead(Ⅱ) adsorption.Neither of the old adsorbents for lead(Ⅱ)has the uptake capacity over 2000 mg·g~(-1).The model of pseudo-second-order describes well the process kinetics.The adsorption process of lead(Ⅱ) is independent of temperature changes.This compound can adsorb lead(Ⅱ) from tap water.In addition to introducing a new MOF with the highest uptake capacity for removal of Pb(Ⅱ) that is the outright novelty of this study,the concurrent modeling of both the removal percent(R) and the uptake capacity(q) is another important advantage.Because it achieves the more economical and favorable optimum conditions in comparison with the single optimization of each response.     

Adsorption of Methyl Orange on Magnetically Separable Mesoporous Titania Nanocomposite☆

The adsorption of mesoporous Fe3O4–SiO2–TiO2 (MFST), which can be separated easily from solution by a mag-net, for the removal of methyl orange (MO) was investigated. The nitrogen adsorption–desorption...     

Superhigh selective capture of volatile organic compounds exploiting cigarette butts-derived engineering carbonaceous adsorbent

Herein, we develop cost-efficient superhigh-performance of engineering carbonaceous adsorbent from cigarette butts using combined wet-impregnated and re-dispersed method of KOH, which optimizes the implant approach of activator, breaking the restriction of selective capture of toluene using traditional activated carbon. The Brunauer-Emmett-Teller (BET) surface area and pore volume of targeted adsorbent can attain 3088 m²·g^-1 and 1.61 cm³·g^-1, respectively, by optimizing the temperature-dependent synthetic factor effect of the adsorbent. The adsorption capacity of resultant adsorbent for presenting volatile benzene and toluene shows a positive correlation with increasing carbonization temperature of carbon precursor. Besides, we demonstrated the unsmoked and smoked butts derived adsorbents afford feeble difference in saturated adsorbed capacity of volatile organic compounds (VOCs). The highest adsorption capacity of sample CF-800 for benzene and toluene in CF group is as high as 1268.1 and 1181.6 mg·g^-1 respectively, slightly higher than that of sample UF-800, but far outperforming reported other adsorbents. The predicted adsorption selectivity of CF-800 and UF-800 for C₇H₈/H₂O (g) using the DIH (difference of isosteric heats) equation reach up to ca. 3800 and 7500 respectively, indicating the weak adsorbability of water vapor on the developed adsorbent and greater superiority of the smoked butts derived adsorbents in selective capture of VOCs at low relative humidity in the competitive adsorption process for practical mixed VOCs.     

CO2-hierarchical activated carbon prepared from coal gasification residue: Adsorption equilibrium,isotherm, kinetic and thermodynamic studies for methylene blue removal

Mineral matter in a residue(RC G) from coal gasification(CG) was removed by two-stage acid leaching. Hierarchical activated carbon(HAC) was prepared by activating RC Gwith CO_2. The performance of HAC on removing methylene blue(MB) from an aqueous solution was investigated. HAC was characterized by N_2 adsorption–desorption isotherm, Fourier transform infrared spectroscopy, and scanning electron microscopy. The results show that HAC exhibits hierarchical pore structure with high specific surface area(862.76 m~2·g~(-1)) and total pore volume(0.684 cm~3·g~(-1)), and abundant organic functional groups. The adsorption equilibrium data of MB on HAC are best fitted to the Redlich-Peterson. The kinetic data show that the pseudo-first-order model is more suitable at low MB concentration, while the advantages of the pseudo-second-orderand the Elovich models are more obvious as the concentration increases. According to the thermodynamic parameters, the HAC-MB adsorption process is spontaneous and endothermic.     

A high-performance biochar produced from bamboo pyrolysis with in-situ nitrogen doping and activation for adsorption of phenol and methylene blue

Nitrogen doping is a promising method for the preparation of functional carbon materials. In this study, a nitrogen-doped porous coral biochar was prepared by using bamboo as raw material, urea as nitrogen source, and KHCO³ as green activator through in-situ pyrolysis. The structure of the obtained biochar was characterized by various techniques including nitrogen adsorption and desorption, Raman spectroscopy, X-ray photoelectron spectrometer, and etc. The adsorption properties of nitrogen-doped biochar were evaluated with phenol and methylene blue probes. The results showed that the nitrogen source ratio had a significant effect on the evolution of pore structure of biochar. Low urea addition ratio was beneficial to the development of pore structures. The optimum specific surface area of nitrogen-doped biochar could be up to 1693 m²·g^-1. Nitrogen doping can effectively improve the adsorption capacity of biochar to phenol and methylene blue. Biochar prepared at 973.15 K with low urea addition ratio exhibited the highest adsorption capacity for phenol and methylene blue, and the equilibrium adsorption capacity was 169.0 mg·g^-1 and 499.3 mg·g^-1, respectively. By comparing the adsorption capacity of various adsorbents in related fields, it is proved that the nitrogen-doped biochar prepared in this study has a good adsorption effect.