Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 20
·10766-10775
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IF 11.9
Nan Zou,Jie Chen,Ting Qiu,Ying Zheng
Direct hydrogenation of CO2 to ethanol is a highly economical carbon reduction strategy. However, the CO2 hydrogenation process traditionally requires high temperatures, typically higher than 300 °C, to activate CO2 molecules, which is unfavorable to the formation of ethanol. In contrast, we applied the novel non-thermal plasma to activate CO2 at ambient conditions and a Cu(I)-MOF catalyst to selectively synthesize ethanol for the selective transformation of CO2 into ethanol. The best catalyst, Cu(I)-HKUST-17.5, achieved 41.2% CO2 conversion and up to 62.9% ethanol selectivity under ambient conditions. The control experiments indicated that the Cu(I) sites are key to realizing C–C coupling and ethanol synthesis. An unreported synergistic catalytic mechanism between non thermal plasma and the Cu(I) and Cu(II) sites on the catalyst is proposed based on the DRIFTS analysis. Overall, our work confirms the feasibility of utilizing non thermal plasma assisted catalysis for the selective conversion of CO2 to ethanol under mild conditions.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yonghou Xiao,Qiang Guo,Shuohan Yang,Qidong Zhao,Gaohong He
The cuprous-ion-based zeolites constructed by introducing Cu(I) adsorption active sites into zeolite Linde Type A have proved to be efficient in carbon monoxide (CO) adsorption with high selectivity and capacity. However, how to directly fabricate zeolite 4A containing copper species and effectively overcome cuprous ion aggregation during the preparation process is still a challenge. Here, we propose an efficient fabrication method to synthesize highly dispersed Cu(I)-modified octahedral zeolite 4A adsorbents using a molecular complex formed by a hydrogel with a silicon/aluminum molar ratio of 1:1, copper ions, and tetramethylammonium hydroxide (TMAOH) as the template. Zeolite 4A containing copper ions was directly obtained by incorporating the precursor of cuprous ions into the confined space between zeolite 4A channel walls and TMAOH. The target zeolite Cu(I)/4A adsorbent with highly dispersed Cu(I) was constructed after introducing VCl3 as the reducing agent via the solid-state dispersion method during the process of removing the template. In comparison with pristine zeolite 4A, a bimodal microporous pore size distribution was observed in as-synthesized Cu(I)/4A. Cu(I)/4A exhibited an enhanced static (1.15 mmol/g) and dynamic (0.0016 mmol g−1) CO adsorption capacity, respectively, at 25 °C and 1 bar. Moreover, Cu(I)/4A displayed a lower H2 adsorption capacity under identical conditions. Through calculation using the ideal adsorption solution theoretical (IAST) equation, the CO selectivity from the CO/H2 mixture on Cu(I)/4A attained ca. 16.95. Therefore, Cu(I)/4A with highly dispersed Cu(I) was successfully fabricated, and its excellent CO adsorption selectivity and capacity enable it to be potentially applied for the actual deep separation of CO/H2.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2020
·
IF 4.335
Lujia Mao,Chunlei Li,Libo Xiang,Dejun Fu,Wangyang Ma,Qing Ye
The synthesis of allenyl-Bdan has been realized via the Cu(I)-catalyzed borylation of propargylic alcohols. This methodology offers a facile and efficient pathway toward allenyboronates with diverse functional groups due to the simple access to the substrates. The substrates bearing ester groups are well-tolerated in the synthesis of allenyl-Bdan under the Lewis acidic conditions. The structures of two allenyl-Bdan were further confirmed via single-crystal X-ray diffraction.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yichen Ding,Dongya Li,Shiyu Zuo,Zeyu Guan,Su Ding
The synergistic effect of radicals and non-radical pathways has attracted much attention for pollutant removal in complex water environments. A novel B-doped CuO/Cu 2 O composite material (B-Cu x O) was synthesized to activate PMS for the degradation of bisphenol A (BPA). XPS and FT-IR proved that B was doped into the Cu x O, which changed the proportion of Cu(Ⅱ) and Cu(Ⅰ). As a result, the cycle of Cu(Ⅱ)/Cu(Ⅰ) was promoted and the kinetic degradation rate of BPA increased by 12 times. The radicals quenching experiments and EPR verified the effects of radicals (·OH and SO 4 ·- ) and non-radical ( 1 O 2 ) pathways in the pollution degradation processes. The results show that B doping accelerated the Cu(Ⅱ)/Cu(Ⅰ) cycle, and at the same time realized the synergistic effect of radicals and non-radical. The PMS/B-Cu x O system exhibited consistent performance in a wide pH range of 5–11. The toxicity evaluation of the transformation products among BPA solutions was studied. This study provided a novel method for accelerating the catalysis of radicals and non-radical synergy.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 19
·8930-8939
·
IF 9.931
Yu-Xia Li,Shuai-Shuai Li,Ding-Ming Xue,Xiao-Qin Liu,Meng-Meng Jin,Lin-Bing Sun
Cu(I)-containing materials have great potential in various applications such as in CO adsorption; however, development of an efficient and controllable method to produce Cu(I) sites remains a significant challenge; herein, a two-step double-solvent (DS) strategy is reported for the first time to fabricate Cu(I) sites in a representative metal–organic framework, MIL-101(Cr); this strategy ensures that both introduction of the Cu(II) precursor and its reduction to Cu(I) occur inside the pores and significantly minimizes the aggregation of Cu species. This is difficult to realize through conventional methods used for Cu(II) introduction (wet impregnation) or reduction (liquid-phase reduction). The two-step DS strategy involves selective reduction of Cu(II) to form Cu(I) without the formation of any Cu(0). The obtained Cu(I)-containing materials exhibit an excellent CO adsorption capacity (up to 2.42 mmol g−1) at 298 K and 1 bar, much better than that of the benchmark adsorbents including CuCl/γ-Al2O3 (1.0 mmol g−1), CuCl/MCM-41 (0.57 mmol g−1), and CuZSM-5 (0.11 mmol g−1).
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Xiaoying Gao,Yunjia Liu,Ke Zhang,Jinlan Weng,Rongqing Chen,Xiaoyi Zhang,Zhipeng Wang,Shenghong Yang,Jian Liu
External light stimuli strategy under conventional conditions achieves a sustainable future due to its controllable spatial and temporal precision coupled with environmental friendliness. Herein, atomic Cu(I)-carbon nitride (Cu-CN) was synthesized and served as specific light-stimuli oxidase mimics for total antioxidant capacity (TAC) assay. Singlet oxygen (1O2) and hydroxyl radical (·OH) are the main intermediates, which can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) into its blue oxidant and therefore improve photothermal signal generation. Based on the intrinsic light responsiveness and photothermal conversion property, we established a colorimetric and photothermal dual-mode sensing platform. The proposed dual-mode assay presented a specific assay of ascorbic acid with LOD of 0.28 μM and 0.15 μM, respectively. This platform was further successfully applied to assess TAC of fruits and beverages. It is believed that the intelligently modulated activity and dual-mode detection function of such atomic enzyme mimics can offer a promising strategy for other analytical assays in high repeatability and reproducibility.
研究领域:
生物化学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2018
·
IF 1.703
Jiajia Lai,Xianying Duan,Hui Yang,Meilin Wei
Two proton-conductive Cu(I) complexes based on Keggin-type clusters, [Cu(debqdc)2]2[HPW12O40]·4H2O (1), and [Cu(debqdc)2]2[HPW12O40]·debqdc·4H2O (2), where debqdc is diethyl 4,4′-dicarboxy-2,2′-biquinoline, were simply synthesized at room temperature. The products were structurally characterized by elemental analyses, infrared spectroscopy, and single-crystal X-ray diffraction analyses. Single-crystal X-ray diffraction analyses revealed that both complexes crystallized in the triclinic space group P−1 and presented two three-dimensional supramolecular networks with one-dimensional hydrophilic channels via hydrogen-bonding interactions and π–π stacking interactions between the aromatic rings. In the [Cu(debqdc)2]+ ion, debqdc acts as a bidentate nitrogen donor ligand in the chelating fashion. The bulky debqdc ligand constrains the Cu(I) metal center within such a rigid environment in a tetrahedral geometry. The two complexes exhibit good proton conductivities (10−5 ~ 10−4 S cm−1) at 100 °C in the relative humidity range 35 ~ 98%. The luminescence behaviors of these complexes in the solid state at room temperature have also been investigated. Upon excitation at 285 nm, both 1 and 2 display three main emission peaks centered at 470, 520, and 568 nm, respectively.
研究领域:
材料科学
·
晶体化学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 21
·6416-6426
·
IF 6.177
Binxiong Guang,Wei Zhang,Yiwei Zhang,Yahui Xiao,Yong Liu
A novel, efficient and economical process of cyclohexanol (CHOL) production based on cyclohexene esterification–hydrogenation has become a research hotspot in recent years. Wherein, hydrogenation of cyclohexyl acetate (CHA) derived from the esterification of cyclohexene with acetic acid is a crucial step. Combining the advantages of metal complexes and heterogeneous catalysts, the robust Cu(I) coordinated amino-functionalized poly(ionic liquid)s (PILs-Cu(I)) were, in this research, synthesized for use in the mild and highly selective hydrogenation of CHA to CHOL. The results of FT-IR, UV-vis, BET, XPS and SEM-EDS confirmed that the Cu(I) was dominant in the PILs-Cu(I), and was homogeneously and stably coordinated on the amino-functionalized poly(ionic liquid)s. Benefiting from that, the PILs-Cu(I) was endowed with an unprecedented performance in the mild and highly selective hydrogenation of CHA to CHOL. Specifically, 95.6% CHA conversion with 96.6% selectivity of CHOL, and 97.0% selectivity of ethanol was obtained under extremely mild conditions of 80 °C and 2 MPa H2. Furthermore, no significant activity loss was observed over the PILs-Cu(I) after recycling for at least five times, delivering excellent stability and reusability.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Shuohan Yang,Yonghou Xiao,Wuyue Zhang,Yu Qiao,Qidong Zhao,Ning Zhang,Gaohong He
Cuprous ion-based zeolites have been proven as promising carbon monoxide (CO) adsorbents by virtue of their excellent adsorption and regeneration properties due to π complexation. However, existing preparation methods still suffer from the problems of a cumbersome process and low loading amounts of cuprous ions. Herein, we proposed a one-step synthesis strategy of using ethanol as a solvent to provide a reducing protective environment, which enabled the facile and controllable preparation of highly dispersed CuCl over 5A zeolites. Using CuCl as a copper source, to ensure the integrity of the 5A zeolite structure, CuCl species were directly loaded onto the 5A support in one step. Ethanol solution could effectively protect Cu(I) from being oxidized by oxygen in air and improve the stability of cuprous ions in Cu(I)/5A adsorbents. The results demonstrated that the Cu(I)/5A prepared by this method exhibited a superior CO adsorption performance to the pristine 5A zeolite. The adsorption capacity of CO over Cu(I)/5A attained 3.44 mmol·g–1 at 298 K and atmospheric pressure, which was evidently superior to those of CuY (2.7 mmol·g–1) and CuSAPO34 (1.84 mmol·g–1) reported in the literature, while the adsorption capacity of H2 was only 0.069 mmol·g–1 under the same condition. According to the ideal solution adsorption theoretical model, CO was preferentially adsorbed and the IAST selectivity of CO in the CO/H2 binary mixture over Cu(I)/5A was about 273.4. This study provides a novel and effective way to synthesize high-efficiency CO adsorbents.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Li Fu,Bin Zhang,Xiaoyan Long,Kena Fu,Xuwen Gao,Guizheng Zou
Screening a novel electrochemiluminescence (ECL) system is crucial to ECL evolution. Herein, an efficient ECL system with less interference and environmental concern under physiological condition is developed via a unique internal Cu(I)/Cu(II) couple cycling amplified strategy by employing the glutathione- and citrate-capped copper indium sulfide (CIS)/ZnS nanocrystals (NCs) as electrochemiluminophore and N2H4·H2O as co-reactant. CIS/ZnS NCs can be electrochemically injected with valence band (VB) hole at 0.46 and 0.87 V (vs Ag/AgCl), and then achieve the same hole-injected states by relocalizing VB holes with the Cu(I) species inside of CIS/ZnS NCs to form internal Cu(II) defects, while each N2H4·H2O molecule can be successively oxidized to two more reducing species N2H3• and N2H2 around 0.10 V, and inject conduction band (CB) electron onto CIS/ZnS NCs for triple times. The internal Cu(I)/Cu(II) couple cycling involved radiative-charge recombination between these VB hole and CB electron eventually enables two efficient near-infrared ECL processes (around 731 nm) at 0.55 and 0.87 V, in which each single nanocrystal may participate in multiple ECL reaction cycles to produce multiple photons for amplified ECL, similar to the tris(bipyridyl)ruthenium(III) based ECL system. The low-triggering-potential ECL process at 0.55 V can be utilized to selectively determine Cu(II) with a wide linear range from 10 and 1500 nM and a limit of detection of 5 nM (S/N = 3). This work presents a NCs engineering and co-reactant selecting combined strategy for further ECL evolution.
研究领域:
分析化学
·
纳米技术
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2021
·Vol. 8
·期 9
·2618-2628
·
IF 8.131
Ting Chen,Zhiliang Zhu,Yujie Bao,Hua Zhang,Yanling Qiu,Daqiang Yin
The effective construction of electron transport channels has essential significance for electron-transfer rate enhancement in REDOX processes during peroxymonosulfate (PMS) activation. This study focuses on the establishment of Cu-involved covalent bonds due to the unique electron configuration of Cu ions. The strategy was achieved by anchoring Cu atoms to an O-doped g-C3N4 (Cu–O–CN) matrix. The C–O–Cu linkage was successfully constructed, derived from the precise incorporation of oxygen. From XAFS, H2-TPR, and solid-ESR characteristic observations, the desired REDOX performance was verified. The constructed C–O–Cu linkages were treated as electron transport channels for electron transfer while reacting with PMS, effectively accelerating the REDOX circulation of the Cu(II)/Cu(I) redox couple and promoting the consecutive generation of active species. Consequently, nearly 100% bisphenol A (BPA) was degraded in the Cu–O–CN/PMS reaction system within 30 min. This demonstrates the effectiveness of Cu–O–CN for PMS activation. The prepared Cu–O–CN exhibited definite stability and potential reusability. This research not only highlights the tailored design of heterogeneous catalysts for PMS activation but also broadens its application in water purification.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Qiang Le,Zan Liu,Zhilin Cheng
In this work, a novel core-shell nanostructured coaxial nanofiber membranes (CFMs) were successfully produced by the coaxial electrospinning . The structure and composition of CFMs were probed by a series of characterizations. The results demonstrated that the CFMs were comprised of the versatile core-shell structure nanofibers, therein Cu(I)/UIO-66 scattered in the shell layer and HNTs dispersed in the core layer. As applied in the selective adsorption desulfurization , the Cu(I)/UIO-66 embedded on the surface of the nanofiber undertook the adsorption active sites, while HNTs in core layer served as enhancing the mechanical performance of PAN nanofibers. The CFMs had the superior adsorption performance in the batch adsorption (maximum:40.14 mg·g −1 ) and fixed-bed adsorption (maximum: 47.43 mg·g −1 ) capacities for benzothiophene (BT) from fuel oil, respectively. Furthermore, due to having the robust mechanical performance, the CFMs exhibited the preferable recycling adsorption and mechanical stability . The adsorption mechanism of BT molecules on CFMs was explored by the kinetics, isotherms and thermodynamic models , indicating the existence of the synergistic effect of physical adsorption and chemical adsorption.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
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