ENVIRONMENTAL TECHNOLOGY
·
2014
·
IF 1.197
Rui-tang Guo,Wen-long Zhen,Wei-guo Pan,Jie-nan Hong,Qiang Jin,Cheng-gang Ding,Shi-yi Guo
CeO2–CuO/Al2O3 catalysts were prepared by three different methods and their activities for selective catalytic reduction (SCR) of NO with NH3 were investigated. As can be seen from the experimental results, the catalyst prepared by the single-step sol–gel (SG) method showed the best SCR activity and resistance to SO2 and H2O. In order to investigate the relationship between the preparation method and the performance of SCR catalysts, the catalysts were characterized by using Brunauer–Emmett–Teller, X-ray diffraction, temperature programmed reduction with hydrogen, temperature programmed desorption with ammonia, X-ray photoelectron spectroscopy, Fourier transform infrared and thermo-gravimetric analysis techniques. It was found that the excellent performance of CeO2–CuO/Al2O3 catalyst prepared by the single-step SG method should be resulted from its large surface area, low crystallinity, high oxygen storage capacity, high NH3 adsorption capacity, high concentration of surface chemisorbed oxygen, weak sulphation process and weak water absorption.
研究领域:
环境科学
·
催化材料科学
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yanpeng Chen,Xing Zhu,Kongzhai Li,Yonggang Wei,Yane Zheng,Hua Wang
Syngas generation via thermochemical H2O–CO2 splitting relies heavily on a high-temperature decomposition of metal oxides into a reduced state. Meanwhile, typical chemical looping partial oxidation of methane to syngas suffers from the carbon deposition and the low selectivity toward syngas. To overcome these drawbacks, the partial oxidation of methane and H2O–CO2 splitting are coupled to consist of an alternative chemical looping redox scheme for the generation of Fischer–Tropsch (F–T)-ready syngas. The usability of lattice oxygen in a redox catalyst is facilitated, and its redox property is also thermodynamically optimized by using H2O and CO2 as soft oxidants, guaranteeing an effective generation of syngas from both redox steps. The carbon tolerance is greatly enhanced due to H2O or CO2 gasification in the reoxidization step. Experimental studies confirm the redox scheme by using CeO2–LaFeO3 redox catalyst, demonstrating generation of syngas with an H2/CO molar ratio around 2.0 in both methane partial oxidation and H2O–CO2 splitting steps over 30 repeated cycles at 850 °C. A syngas selectivity of 95% in methane partial oxidation and nearly 100% conversion of CO2 to CO can be achieved. Synergistic effect and competing reaction between H2O and CO2 splittings over the reduced redox catalyst are the key factors for the control of syngas composition and the intensification of CO2 splitting. The proposed approach can potentially be applied for production of F–T-ready syngas with an increased yield without the need for gas separation when compared to the state-of-the-art thermochemical splitting or methane chemical looping partial oxidation processes.
研究领域:
能源科学
·
化学工程
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2019
·Vol. 30
·期 8
·7950-7962
·
IF 2.195
Hu Bingbing,Guo Qiang,Wang Kang,Wang Xitao
In this paper, a series of indium oxides were prepared by calcining the In(OH) 3 precursors, which were synthesized by hydrothermal method using the mixed solution of ethylenediamine (En) and water as a solvent. The morphologies, particle sizes, pore structure, crystallinity and surface defect concentration of these photocatalysts were adjusted by varying the ratio of En to water during the preparation of In(OH) 3 precursors. The results revealed that In 2 O 3 photocatalysts obtained from the precursor prepared in En containing solvent exhibited much higher photocatalytic activities for CO 2 reduction with H 2 O when compared to that derived from the precursor prepared in pure water. This result can be ascribed to several reasons as following. Firstly, the En addition with a suitable amount can improve the crystallinity of In 2 O 3 and decrease the surface defect concentration, which obviously depressed the recombination of photogenerated electrons and holes. Also, the addition of En during the preparation of precursor can decrease the particle size, increase specific surface area and pore structure, resulting into the increase of active sites. Finally, the band gap of In 2 O 3 can be slightly narrowed after the addition of En, resulting in enhanced light absorption in the visible region. When the ratio of ethylenediamine to water is 1:1, the as-prepared In 2 O 3 possessing the largest specific surface area and pore volume, enhanced light absorption ability and higher hole–electron separation efficiency, exhibited the highest photocatalytic activity. Under visible light irradiation, the H 2 , CO and CH 4 production rates of 5.3, 8.3 and 27.2 µmol/g cat /h can be achieved, respectively.
研究领域:
材料科学
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环境科学
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DOI
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ACS Catalysis
·
2026
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IF 13.6
Suiyang Dai,Jiahua Luo,Yuhan Zhou,Xin Liu,Yechao Su,Yabo Bian,Xueyan Sun,Ferenc Lónyi,Hongliang Li,Yongzhi Zhong,Jie Zeng
Ammonium bicarbonate (NH4HCO3) is a widely used nitrogen fertilizer that simultaneously offers nitrogen and carbon while consuming CO2 during its synthesis. Conventional NH4HCO3 production relies on the Haber−Bosch process to generate NH3 followed by CO2 neutralization, resulting in high pressure operating conditions (400−500 °C, 100−200 bar). Herein, we present a cascade plasma-thermal catalytic route that converts N2, H2O, and CO2 into NH4HCO3 under atmospheric pressure. In this process, non-thermal plasma activates N2 and H2O to generate NO and H2, bypassing thermodynamic constraints. The plasma-derived NO is then hydrogenated over Pt/HZSM-5 with supplementary H2 from water electrolysis to produce NH3. Finally, simultaneous CO2 absorption leads to the in situ formation of NH4HCO3, achieving a yield rate of 114.5 mmol h–1 at a discharge current of 0.4 A. This integrated approach offers a pathway for nitrogen fertilizer synthesis from air and water, representing a step toward carbon−nitrogen cycle coupling.
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AICHE JOURNAL
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2026
·
IF 4.4
Xin Ta,Qiang Sun,Min Xiao,Zhiwu Liang,Hongxia Gao
Phase-separating absorbents show promise for reducing energy consumption, as desorption requires heating only the CO 2 -enriched phase. This study investigates triethylene glycol monobutyl ether (TGBE) as a phase-separation promoter for the N-methylaminoethanol (MAE)–water system. The role of TGBE in restructuring hydrogen-bond networks and promoting rich-phase aggregation was analyzed using gas–liquid–liquid equilibrium, 13 C NMR, gas chromatography, and molecular dynamics (MD) simulations. Experimental results demonstrate that TGBE significantly reduces rich-phase volume while achieving CO 2 equilibrium loadings of 3.59 mol/kg for water-containing systems and 4.73 mol/kg for water-free systems. MD simulations reveal that CO 2 absorption redistributes intermolecular interactions, where strengthened hydrogen bonds between water and ionic species drive polar rich-phase aggregation. Furthermore, an empirical model, a GBDT-based predictive model, and a modified Deshmukh–Mather framework were developed to describe phase behavior with AARDs of 2.81%, 4.58%, and 6.61%, respectively. These findings provide a theoretical foundation for designing energy-efficient CO 2 capture systems.
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ChemSusChem
·
2022
·Vol. 15
·期 24
·e202201739
·
IF 9.14
Kang Zhou,Nan Wang,Xuan Qiu,Haijiao Xie,Peng Wei,Xiaoli Dong,Yonggang Wang
Graphical No water, no problem : The H 2 O activity in aqueous electrolyte is restrained by adding glycerol and acetonitrile into the electrolyte to form hydrogen bonds between organic solvents and H 2 O molecules, which facilities the smooth Zn deposition and alleviates Zn corrosion. Therefore, the Zn//Zn symmetrical cell cycles for over 1300 h and the Zn//FD28 full cell cycles for 9000 cycles. The advantages of low cost and high safety of zinc (Zn) metal have attracted much attention on its application in batteries, but H 2 O-induced issues of hydrogen evolution reaction (HER), Zn corrosion, and Zn dendrites formation limit the application. Here, a strategy of adjusting H 2 O activity was provided by adding glycerol (GL) and acetonitrile (AN) into aqueous electrolyte to form hydrogen bonds between organic solvents and H 2 O, which alleviated the Zn corrosion. Furthermore, molecular dynamics (MD) simulation indicated that GL could exclude H 2 O from the Zn 2+ solvation shell, thus preventing undesired HER and Zn dendrites formation. Therefore, the corresponding Zn//Zn symmetrical cell showed a ultralong lifespan (1300 h). Then, a Zn-organic battery with 3,7-dimorpholino-phenothiazin-5-ium iodide (FD28) cathode was fabricated by using such electrolyte. Interestingly, the reduced H 2 O activity also ensured the stable operation of organic cathode, and thus the full cell showed superior cycle stability for over 9000 cycles (≈1100 h), which is superior to previous reports. Moreover, such electrolyte owns novel properties of nonflammability, great weatherability, and low freezing point, thus boosting the practicality of the battery.
研究领域:
材料科学
·
电化学
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 14
·4423-4428
·
IF 4
Xue-Ying Zhang,Xiao-Han Zhang,Bing-Ping Yang,Jiang-Gao Mao
A new alkaline earth–rare earth iodate, Ba2Ce(IO3)8(H2O), has been synthesised by a hydrothermal method and its structure has been determined by single-crystal X-ray diffraction. Ba2Ce(IO3)8(H2O) crystallises in the polar space group Pna21 (No. 33) with unit cell parameters of a = 15.5042(5) Å, b = 7.8841(3) Å, c = 19.5359(8) Å, V = 2388.00(15) Å3, and Z = 4. The structure of Ba2Ce(IO3)8(H2O) is characterised by zero-dimensional (0D) [Ce(IO3)8(H2O)]4− units separated by Ba2+ cations. Large crystals of Ba2Ce(IO3)8(H2O) with dimensions of a few millimetres have been grown. The UV-vis-NIR transmission spectroscopy measurements of the compound showed that it has a short wavelength absorption edge at 381 nm. Ba2Ce(IO3)8(H2O) exhibits a relatively weak second-harmonic-generation (SHG) response, about 0.2 times that of KDP, which is mainly due to the fact that the polarisation effects of the IO3 groups in the structure largely cancel each other out. The relationships between the structure and the physical properties of Ba2Ce(IO3)8(H2O) have also been calculated theoretically. Ba2Ce(IO3)8(H2O) has a band gap of 2.44 eV, which is determined by the Ce–O and I–O interactions and is larger than those of many simple metal iodates. The introduction of alkaline earth metals favours an increase in band gap. Our work shows that the SHG and birefringence properties are closely related to the arrangement of the functional groups in the compounds.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Shen Zhang,Caidi Jin,Kuichuan Sheng,Ximing Zhang
5-hydroxymethylfurfural (HMF) primary can be synthesized from monosaccharides including glucose and fructose, cost is one of barriers to realize HMF large-scale production. In this study, a high HMF yield of 69.6 mol% was obtained at 180℃ for 5 min using biomass derived cellulose formate as reactant, which was prepared by formylation of cellulose using recyclable formic acid, and sequentially catalyzed by hydrochloric acid (HCl) and aluminum chloride (AlCl 3 ) in dimethyl sulfoxide (DMSO) and H 2 O system. To investigate the effect of cosolvents and formyl groups on the cellulose formate conversion, kinetics analysis and molecular dynamics simulations were conducted. Reaction kinetics study shows that the rate constant of hydrolysis of cellulose formate to glucose increased by almost three times in DMSO-H 2 O and the reaction rates’ constants of glucose, fructose and HMF to humins decreased with the presence of DMSO. Molecular dynamics simulations show that formyl group and DMSO increased its hydrophilicity around the reactive hydroxyl group on the carbon ring and steric hindrance of formyl group affect the distribution of water molecular and DMSO molecular around formylated glucose, resulting in facilitating the formation of a precursor to fructose and inhibiting the formation of humins during formylated glucose conversion.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Cao Cheng,Hongyan Zhang,Fan Li,Shuguo Yu,Yan Chen
In this study, a gas sensor based on TiO 2 /WO 3 ·H 2 O (TW) heterojunction with high sensitivity, excellent selectivity and long-term stability for ammonia (NH 3 ) detection was successfully prepared by hydrothermal method . Compared with WO 3 ·H 2 O and TiO 2 , TW heterojunction shows excellent selective to NH 3 and the response varies by 3 orders of magnitude to 500 ppm NH 3 at room temperature (RT, 25 ± 3 °C). The lowest response limit of TW is 0.5 ppm and the response/recovery time is 2.35 s/1.95 s. The main reason for improving the performance of TW heterojunction to NH 3 detection is that TiO 2 nanoparticles cause more oxygen free radicals on the surface of TW heterojunction, which can react with more NH 3 molecules to release more electrons. Therefore, heterojunction structure increases the electrons and reduces the width of electron depletion layer in TW gas sensor. In addition, TW heterojunction has small and uniform particle size which can provide more active sites for the reaction between NH 3 and oxygen free radicals to release more electrons. This work provides a heterojunction structure composed of TiO 2 and WO 3 ·H 2 O to effectively improve the performance of sensor for NH 3 detection at RT, which is beneficial to the development of high-performance gas sensors.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ren Yuqi,Fu Yiwei,Li Naixu,You Changjun,Huang Jie,Huang Kai,Sun Zhenkun,Zhou Jiancheng,Si Yitao,Zhu Yuanhao,Chen Wenshuai,Duan Lunbo,Liu Maochang
H 2 O dissociation plays a crucial role in solar-driven catalytic CO 2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO 2 catalyst with single-atom Ni anchored around its surface V o sites by replacing Ce atoms to promote H 2 O dissociation and achieve effective photothermal CO 2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH 4 production and prevents V o from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d -impurity orbitals, thereby inducing more effective H 2 O activation. The catalyst presents a CH 4 yield of 192.75 µmol/cm 2 /h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H 2 O-activating catalysts for CO 2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Guangfei Qu,Qian Zhao,Ronglong Jian,Junya Wang,Dianxin Liu,Ping Ning
Beginning with the formation of the ionic liquid/water two-liquid phase catalytic system for absorption of PH 3 , we designed and synthesized Cu + -[Bmim]PF 6 , which has a hydrophobic property, and later formed a two-liquid phase system with Cu + -[Bmim]PF 6 and water, which has high PH 3 absorption efficiency, and an effective separation of the product and the catalyst was achieved. The effects of temperature and O 2 concentration on phosphine absorption, and the distribution of catalytic components and products in the ionic liquid/aqueous two-phase system were studied. Moreover, the mechanism of Cu + -ILs/water two-liquid phase catalytic oxidation of phosphine was discussed based on results from the analysis of FT-IR and ion chromatography . The results demonstrated that the optimum oxygen content in the reaction was 3%, and the optimum reaction temperature was 45 °C. Cu + -ILs/water two-liquid phase system has a high absorption efficiency for PH 3 , the absorption process is liquid phase catalytic oxidation and the product is H 3 PO 4 . The two-liquid phase system is semi-intelligent. The system can achieve high performance liquid phase catalytic oxidation of PH 3 , as well as automatic separation of H 3 PO 4 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Li Xu,Qiye Ju,Haiyan Jiang,Na Geng,Jianze Xiao,Ziqian Xue,Tingyu Zhu,Yangyang Guo
Heavy water (D 2 O) electrolysis is the primary technology for D 2 production, playing an irreplaceable role in fields such as nuclear fusion research and isotope tracing. However, the inherent similarity in chemical properties between H 2 O and D 2 O (with only a 1.4 °C difference in boiling points) poses significant challenges to their separation. Furthermore, the extremely low natural abundance of D 2 O (0.015 %) increases the difficulty and cost of separation, while traditional electrolysis and distillation techniques are highly energy intensive. Therefore, there is an urgent need to develop novel adsorbents for efficient and environmentally sustainable H 2 O/D 2 O separation. Herein, we used polydentate ligand 2, 5-dihydroxyterephthalic acid (DOBDC) and its derivatives 4,4́-(anthracene-9,10-diyl) bis (2-hydroxybenzoic acid (ABHB) as raw materials to prepare two novel high coordination Sr-MOFs namely IPE-1 and IPE-2, respectively. These MOFs were applied for efficient separation of H 2 O and D 2 O at room temperature. X-ray diffraction results reveal that one Sr atom in IPE-1 is coordinated with 9 oxygen atoms. This high coordination number results in the formation of ultra-small rectangular pores of approximately 2.5 Å. Adsorption isotherms of N 2 , CO 2 , H 2 O, and D 2 O indicate that the ultramicroporous structure of IPE-1 precludes efficient diffusion of CO 2 and H 2 O molecules into the MOF channels. In contrast, the activated IPE-2 exhibits good CO 2 , H 2 O, and D 2 O uptake capacities of 3 mmol/g, 8.38 mmol/g, and 6.51 mmol/g at 298 K, respectively. The Q st values and K sap values of H 2 O and D 2 O indicate that the adsorption rates of H 2 O were much higher than D 2 O under 0.2 < P/P 0 < 0.7, with a calculated ratio of approximately 1.26. This study not only provides appealing MOFs materials for efficient H 2 O/D 2 O separation at room temperature but also provides a new avenue for preparing adsorbents with high stability and high separation performance.
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