ENERGY
·
2023
·
IF 9
Lijian Jin,Xueyan Hou,Lingxiao Zhan,Dawei Hou,Lina Gu,Daguang Zhang,Jianchong Shen,Zhihao Zheng,Chao Lv,Shaoqing Liu,Linjun Yang
In this study, we examined the impacts of complete and partial substitution of DEEA with physical solvents (n-butanol) on the performance of AEEA/H 2 O absorption, regeneration, and phase separation. The higher hydrophobicity (log P) of n-butanol, as a phase splitter , expedites the separation process from the AEEA-CO 2 product. Through additional refinement of the mass ratio between n-butanol and DEEA, it was observed that substituting a small portion of DEEA with n-butanol had negligible impact on the absorption capacity and enrichment of the enriched phase. However, it significantly reduced the phase separation time between the two solvent phases. Furthermore, an increase in n-butanol concentration can enhance cyclic loading. On the other hand, it reduces the production of AEEACOO − /DEEAH + , which is more stable compared with AEEACOO − /AEEAH + . Molecular dynamics simulations revealed that n-butanol can modulate the reduction of water molecules surrounding AEEA, creating a lower water molecule environment, which improves the absorption rate of the absorbent in the pre-absorption phase. The addition of a low concentration of n-butanol improves the initial absorption rate, phase separation performance, circulation capacity, and further reduces the regeneration energy of the absorption solution without compromising the CO 2 loading and regeneration energy.
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高影响因子
Science China-Chemistry
·
2013
·Vol. 56
·期 11
·1651-1657
·
IF 1.327
Zhao XiJuan,Fang JingMei,Li YuanFang,Huang ChengZhi
Selective recognition of adenosine 5′-triphosphate (ATP) is of great significance owing to its indispensable functions to organisms. Also, it is a challenging task because other nucleosides triphosphate hold the same triphosphate group and structurally planar bases as ATP. It is known that metal-organic frameworks (MOFs) are a new type of sensing material. In this work, highly selective recognition of ATP against other nucleosides triphosphate is successfully achieved with a luminescent MOF of [Zn(BDC)(H 2 O) 2 ]
n
(BDC 2− = 1,4-benzenedicarboxylate). [Zn(BDC)(H 2 O) 2 ]
n
dispersed in water shows a remarkable redshift of the emission wavelength upon addition of ATP, while cytidine 5′-triphosphate (CTP), uridine 5′-triphosphate (UTP), and guanosine 5′-triphosphate (GTP), as well as some inorganic anions such as P 2 O 7
4− or PO 4
3− can’t induce such spectral change as ATP. 1 H NMR, 31 P NMR and Raman spectra indicate that both π-π stacking interactions and the coordination of Zn(II) with adenine and the phosphate group are involved in the interaction of [Zn(BDC)(H 2 O) 2 ]
n
with ATP. In addition, the experimental results showed that the redshift extent of the emission wavelength of [Zn(BDC)(H 2 O) 2 ]
n
has the linear relationship with the concentration of ATP in the range of 0.3–1.8 mmol/L. Based on this, the detection of ATP content in the sample of ATP injection was made with satisfactory results. This system pioneers the application of MOFs in the recognition of nucleotides, and testifies that the participation of base in the recognition process can improve the selectivity against the other nucleotides.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Zihan Zhou,Yunwen Wu,Silin Han,Tao Hang,Huiqin Ling,Jie Guo,Su Wang,Ming Li
3D NAND is one of the most promising storage devices due to its high storage density and low energy consumption. Selective wet etching of Si 3 N 4 by hot-concentrated phosphoric acid (PA) solution is a key process for 3D NAND fabrication. However, the channel material, polycrystalline silicon (poly-Si), is unexpectedly dissolved due to its inevitable exposure to the PA etching solution, which causes device failure and thus limits the stacking density of 3D NAND. Herein, to avoid the detrimental dissolution of poly-Si, we unveil the mechanism of poly-Si dissolution in PA solution from kinetic and thermodynamic perspectives. We find that the etch process shows a two-stage reaction, in which H 2 O plays a key role in lowering the activation barrier for poly-Si etching. Further thermodynamic analysis demonstrates that poly-Si prefers to be oxidized by H 2 O to suboxide rather than to SiO 2 . Combined with surface chemistry characterization, we propose the dissolution mechanism as a two-stage process involving the dissolution of suboxide interface and bulk poly-Si, where the nucleophilic substitution of Si–H with Si–OH on bulk poly-Si surface determines the overall etch rate. This study advances the 3D NAND development by establishing a theoretical foundation for identifying and implementing efficacious strategies to impede detrimental dissolution.
研究领域:
半导体器件
·
材料科学
·
纳米技术
·
化学工程
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2026
·
IF 2.4
Ziyu Zhuang,Manman Zhang,Dandan Gao,Wolfgang Voigt,Dongdong Li,Haitao Feng
Previously, the formation of a stable adduct 2H3BO3·3CsCl (BC) was observed in CsCl(aq) but not in RbCl(aq). The phase equilibria of the H3BO3 + RbCl + CsCl + H2O system were studied to assess the potential for selective separation of Cs from Rb. Solubility isotherms were determined experimentally. Appropriate liquid composition ranges were preselected using modeling with ISLEC’s equilibrium software. Schreinemakers’ wet solid method, XRD, Raman and IR spectra, Roozeboom’s plots, and SEM-EDS were applied to identify the four phase regions H3BO3, 2H3BO3·3(Cs,Rb)Cl (Bss), (Rb,Cs)Cl, and (Cs,Rb)Cl. Notably, in the presence of RbCl, the BC phase incorporates Rb+, forming a substitutional solid solution, Bss, which inhibits selective separation of CsCl. Roozeboom’s plot analysis revealed that RbCl exhibits higher solubility in the Bss phase compared to the (Cs,Rb)Cl solid solution. The separation factor βCs/Rb between the solid Bss phase and the corresponding solution was 2.0, significantly lower than that of (Cs,Rb)Cl (βCs/Rb = 9.5) in the ternary system without H3BO3. This indicates a stronger coordination between CsCl and H3BO3 relative to that of RbCl in the ternary system without H3BO3. The above understanding provides new strategies designing novel B–OH compounds to enhance Cs/Rb separation efficiency in aqueous systems.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2020
·
IF 2.888
Zhan-Ping Qiao,Tian Yang,Shu-Zhi Cao,Yu-Feng Tang,Qi-Chao Yang
Solid-liquid equilibria in the ternary systems RbX + CdX 2 + H 2 O (X = Cl, Br) at T = 298.15 K and under 101.3 kPa were investigated by the method of isothermal solution saturation, and the corresponding phase diagrams were constructed. It was found that there were five crystallization regions corresponding to CdCl 2 ·2.5H 2 O, RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 and RbCl in the system (RbCl + CdCl 2 + H 2 O). Four crystallization regions corresponding to CdBr 2 ·4H 2 O, RbCdBr 3 , Rb 4 CdBr 6 and RbBr were found in the system (RbBr + CdBr 2 + H 2 O). The new solid compounds RbCdCl 3 , RbCdBr 3 and Rb 4 CdBr 6 were congruently soluble in water, and new double salts RbCd 2 Cl 5 ·H 2 O and Rb 4 CdCl 6 were incongruently soluble in water. The new solid-phase compounds RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 , RbCdBr 3 and Rb 4 CdBr 6 were characterized by chemical analysis, XRD and TG-DTG techniques. The standard molar enthalpies of solution of RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 , RbCdBr 3 and Rb 4 CdBr 6 in water were measured to be (20.74 ± 0.16) kJ·mol −1 , (28.00 ± 0.39) kJ·mol −1 , (96.56 ± 0.50) kJ·mol −1 , (35.38 ± 0.33) kJ·mol −1 and (110.64 ± 0.62) kJ·mol −1 by microcalorimetry in the condition of infinite dilution, and their standard molar enthalpies of formation were determined to be −(1545.3 ± 0.6) kJ·mol −1 , −(856.5 ± 0.7) kJ·mol −1 , −(2180.1 ± 1.3) kJ·mol −1 , −(727.1 ± 0.7) kJ·mol −1 and −(1920.5 ± 1.3) kJ·mol −1 , respectively.
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高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2018
·
IF 2.179
Yun-Xiang Ma,Ya-Ping Gong,Chun-li Hu,Jiang-Gao Mao,Fang Kong
Three new d 10 transition metal selenites containing PO 4 tetrahedron, namely, Cd 7 (HPO 4 ) 2 (PO 4 ) 2 (SeO 3 ) 2 ( 1 ), Cd 6 (PO 4 ) 1.34 (SeO 3 ) 4.66 ( 2 ) and Zn 3 (HPO 4 )(SeO 3 ) 2 (H 2 O) ( 3 ), have been synthesized by hydrothermal reaction . They feature three different structural types. Compound 1 exhibits a novel 3D network composed of 3D cadmium selenite open framework with phosphate groups filled in the 1D helical tunnels. The structure of compound 2 displays a new 3D framework consisted of 2D cadmium oxide layers bridged by SeO 3 and PO 4 groups. Compound 3 is isostructural with the reported solids of Co 3 (SeO 3 ) 3-x (PO 3 OH) x (H 2 O) when x is equal to 1.0. Its structure could be viewed as a 3D zinc oxide open skeleton with SeO 3 and HPO 4 polyhedra attached on the wall of the tunnels. They represent the only examples in metal selenite phosphates in addition to the above cobalt compounds. Optical diffuse reflectance spectra revealed that these solids are insulators, which are consistent with the results of band structure computations based on DFT algorithm.
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ENERGY
·
2024
·
IF 9
Tao Tan,Yushu Chen,Yongyue Wang,Zuhao Li,Zhige Zhang,Jun Xie,Yong Chen
The use of green biogas as a raw material for producing methanol-friendly syngas (H 2 /CO ≈ 2) for one-step methanol synthesis has gained significant attention. However, developing efficient catalysts with high activity and stability remains challenging, as they often face issues with stability and carbon deposition. This study presents a Ni/CeO 2 /HT catalyst designed for high activity and long-term stability by leveraging the Ce redox cycle and strong interactions between Ni-CeO 2 and hydrotalcite (HT). The catalyst benefits from abundant oxygen vacancies generated by the Ce 3+ - Ce 4+ pathway, enhancing its ability to activate CO 2 and H 2 O and providing excellent coke resistance. Comprehensive analyses of CO 2 /H 2 O adsorption and carbon elimination mechanisms were conducted using techniques such as in situ H 2 -TPR, CO 2 /H 2 O-TPSR, in situ CH 4 -TPSR, CO 2 /H 2 O-TPO, and FTIR. The Ni/CeO 2 /HT catalyst outperformed others in CO 2 /H 2 O adsorption and CH 4 activation capacity, promoting the generation of active oxygen species and effectively removing coke precursors, thereby improving resistance to Ni sintering and carbon deposition. At 750 °C and a weight hourly space velocity (WHSV) of 32,400 mLg Cat −1 h −1 , it achieved CH 4 and CO 2 conversions of 93 % and 66 %, respectively, with long-term stability exceeding 200 h.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Changhao Wu,Xudong Yu,Nan Zhang,Jing Li,Qi Li,Yousheng Yang,Ke Chen,Bo Yang,Shuang Wang,Yiping Liu,Zhenwen Xing
To solve the massive accumulation of gypsum generated from polyhalite leaching and secondary gypsum, this study investigated phase equilibria of the ternary system NH 4 + , Ca 2+ // SO 4 2- - H 2 O at 323.2 K and 348.2 K. The phase diagrams included 2 invariant points, 3 univariate curves, and 3 crystallization regions corresponding to (NH 4 ) 2 SO 4 , CaSO 4 ·2H 2 O, and double salt koktaite (NH 4 ) 2 Ca(SO 4 ) 2 ·H 2 O. As temperature increased, the crystallization region of CaSO 4 ·2H 2 O contracted, whereas those of (NH 4 ) 2 SO 4 and koktaite expanded, indicating that the temperature-enhanced was beneficial to improve the crystallization efficiency of koktaite. Guided by multitemperature phase diagram, the influencing factors and optimal conditions of the comprehensive utilization process of phosphogypsum were explored. The synthesis of koktaite achieved maximum efficiency under conditions of 1: 1.5 molar ratio, 348.2 K reaction temperature, 90 min duration, and 250 rpm agitation. Concurrently, under solid-liquid ratio of 1: 0.5 and after three leaching cycles of 30 seconds each, the yield of CaSO 4 ·2H 2 O production reached 99.80% with a purity of 99.52%. However, the purity and yield of product decreased due to the accumulation of impurities during the cycles, stabilizing after 6 cycles (koktaite yield: 98.50%; purity: 95.69%; (NH 4 ) 2 SO 4 yield: 97.69%; purity: 95.42%). Granulated koktaite released NH 4 + through layer-by-layer dissolution, which prolonged the dissolution time, and the complete dissolution time was 6 times and 24 times longer than that of ungranulated koktaite and (NH 4 ) 2 SO 4 . This work integrates theoretical phase behavior analysis with process engineering to establish a circular resource recovery strategy for synthesizing high-value products from phosphogypsum.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Xiaoyu Chen,Chenlong Hao,Mengyao Shang,Xiangxin Li,Shuo Wang,Wenming Zhang
Manganese based oxides have significant potential as cathode materials for potassium ion batteries (PIB). Unfortunately, the practical application of manganese-based oxides is hindered by severe electrode surface erosion from electrolyte decomposition products and material expansion and collapse during potassium ion intercalation. Consequently, the surface modification strategy is adopted herein to uniformly cover the surface of K 0.27 MnO 2 ·0.54 H 2 O (KMO) microspheres with LiF/Li x PF y O z coating to effectively protect the electrode surface and significantly inhibit the collapse of the material crystal structure. Additionally, the coating exhibits excellent electron/ion conductivity, enhancing the diffusion efficiency of potassium ions within the electrode material. The existence of LiF/Li x PF y O z coating is confirmed by characterization measurements. The LiF/Li x PF y O z -coated KMO microspheres (sample LLO@KMO-2) exhibit outstanding cyclic stability (66.3 % capacity retention at 50 mA g −1 ) and high discharge capacity (100.2 mAh g −1 at 50 mA g −1 ), demonstrating their excellent cycle stability. The modification strategy of LiPF 6 -electrolyte-solvothermal coating provides an innovative surface modification method for potassium ion batteries , showcasing its potential for application in future high-performance battery technologies.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124167
·
IF 7.5
Chen Chen,Zhenyu Wang,Yasen Li,Jiayao Gao,Xin Chen,Mingjie Jia,Die Shao,Yiming Wang,Xuejian Li,Fuqiang Yu,Guangwen Xu,Junli Xu,Hong-bin Sun
Transition-metal borides have long been developed as promising electrocatalysts for the hydrogen evolution reaction (HER); however, the identity of their true active phase remains controversial. Here, in conjunction with our previous studies, by systematically investigating a series of cobalt- and nickel-boride-derived catalysts through a combined computational and experimental screening, we reveal that HER activity universally originates from the synergistic interaction between metallic sites and hydroxide matrices, enabled by lattice expansion, interfacial electronic transfer, and dynamic surface evolution. As a representative high-performance example, Pt-modified Co(OH) 2 derived from cobalt boride exhibits ultralow overpotentials of 11 mV at 10 mA cm −2 and 95 mV at 500 mA cm −2 , together with long-term stability. Importantly, the same reconstruction principle applies to Ni-boride systems, confirming the generality of this approach. Beyond water electrolysis, we further demonstrate that these HER catalysts are highly effective in Al-H 2 O batteries, where hydrogen evolution is coupled with electrical energy harvest. An alkaline Al-H 2 O battery employing the reconstructed catalyst delivers a power density of 21.96 mW cm −2 . This work establishes that the activity of “boride-based” HER catalysts fundamentally arises from reconstructed metal-hydroxide active centers, providing a development paradigm of transition-metal electrocatalysts.
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DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 24
·8122-8135
·
IF 4.174
Jialin Yu,Qi Gao,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Jianbo Yin,Yuanyuan Zhou,Fangsheng Tao,Yong'an Wang
ε-[Al13O4(OH)24(H2O)12]7+, which shares similarity with the phosphotriesterase active site ZnII–OH–ZnII, was specially chosen to interact with the cluster α-PMo10V2O405− to form a new three-dimensional intercluster, which crystallized in the monoclinic space group P21/m with Z = 2, for the decontamination of chemical warfare agents. The experimental results showed that 50 mg of the compound decontaminated 96.4% (within 120 min) and 99.5% (within 40 min) of sulfur mustard (HD) (4 μL) and soman (GD) (4 μL), respectively, in ambient conditions. The decontamination processes followed first-order reaction kinetics with a rate constant and half-life of 0.01234 min−1 and 56.15 min for HD and 0.1198 min−1 and 5.78 min for GD, respectively. It was concluded that the α-PMo10V2O405− moiety was responsible for the catalytic oxidation of HD into non-toxic sulfoxide, while the ε-[Al13O4(OH)24(H2O)12]7+ moiety was responsible for the catalytic hydrolysis of HD and GD into nontoxic hydrolysates. Besides, the compound showed notable efficacy for the decontamination of HD on guinea pig skin and of GD on Kunming mouse skin, indicating high potential for use in human skin protection and treatment.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xin Liang,Sheng Wang,Jing Zhou,Tengfei Lu,Kaiyu Ruan,Yuqian Xia,Tong Wang
Despite the considerable attention received by switchable solvents in natural product extraction and biorefinery. To tackle this issue, the present study has the following innovative endeavors: (1) Developing an innovative high-speed homogenization assisted extraction method using the DES/SHS/H 2 O system and applying it to the integrated extraction of phenolics, flavonoids, and essential oil from Flos Chrysanthemi Indici . The switching process was characterized using 1 H NMR, the extraction process was optimized employing response surface methodology, the components of extracted essential oils were analyzed by GC–MS, and the cytotoxicity and anti-inflammatory activity of essential oils were determined through MTT and ELISA. Our findings demonstrate that the incorporation of DES can significantly augment the CO 2 switching kinetics of SHS, resulting in a 32.7 % reduction in switching time and a remarkable decrease of 73.7 % residual content within the aqueous phase. The innovative DES/SHS/H 2 O based extraction method exhibited substantial enhancements in phenolics, flavonoids, and essential oil extraction efficiency compared to conventional approaches, yielding extracts with superior chemical profiles and enhanced anti-inflammatory activity. Therefore, the proposed strategy of enhancing the CO 2 switching kinetic properties and extraction ability of SHS by incorporating DES is feasible, providing valuable guidance for the rational design of innovative smart solvent systems. The developed DES/SHS/H 2 O system, exhibiting improved performance, holds significant application and research prospects.
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