CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Siwei Wang,Jin Du,Zhanquan Zhang,Yan Wang,Zhijie Yuan,Yuhan Wang,Tianpei Yi,Fusheng Pan,Zhongyi Jiang
Separating aromatic and aliphatic hydrocarbons can produce high-quality cracking feedstocks and recover value-added aromatic products. Covalent organic framework (COF) may find promising application owing to its exceptional structures and functionalities. In this study, Cu(I)-COF was designed and integrated into Pebax matrix to fabricate facilitated transport membranes. The immobilization of Cu(I) ions onto the COF framework effectively mitigates leaching. Additionally, the COF building blocks provides a stable electron cloud environment for Cu(I), ensuring long-term stability for over 6 months. The vertical channels in the COF afford rapid mass transfer, and the uniformly distributed Cu(I) enhances toluene affinity, thereby intensifying the transfer of toluene. For a 50 wt% toluene/n-heptane mixture, the Cu 3 L 3 -Pa-Pebax-2 membrane demonstrated a permeation flux of 1100 g·m −2 ·h −1 and a separation factor of 5.44. This study provides a new example for the application of multifunctional organic framework materials to fabricate facilitated transport membranes.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Sai-Li Zheng,Yonghe He,Xiao-Kang Qiu,Yuan-Hui Zhong,Lai-Hon Chung,Wei-Ming Liao,Jun He
A novel metal-organic framework [CuCN(TMBP)·H 2 O] n ( TCuCN ) has been synthesized by the reaction of 3,3′,5,5′-tetramethyl-4,4′-bipyrazole (TMBP) and CuCN. Its structure was determined by single-crystal X-ray diffraction (SCXRD) analysis and further characterized by power X-ray diffraction (PXRD) analysis, FT-IR spectroscopy and thermogravimetric (TG) analysis. Previously reported structurally analogous TCuCl , TCuBr , TCuI have also been synthesized for Br 2 adsorption comparison. All of these four MOFs exhibited reversible uptake of Br 2 vapor judging by the unchanged PXRD patterns . Among four MOFs, Br 2 -loaded TCuI showed the most uptake amount of Br 2 (15.7 wt%), providing the formula to be TCuI ·0.33Br 2 . The different uptake amount of Br 2 for TCuX (X = CN, Cl, Br, I) should be mainly ascribed to the intermolecular interaction between CuX and Br 2 .
研究领域:
无机化学
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材料化学
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配位化学
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多孔材料
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气体吸附
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Nano Research
·
2023
·Vol. 16
·期 7
·8827-8835
·
IF 9.9
Wang Xin,Miao Ming,Tang Bowen,Duan Haotian,Zhu Fulong,Zhang Huigang,Zhang Xian,Yin Wen-jin,Fu Yongzhu
Electrochemical conversion of CO 2 (CO 2 RR) into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality. The synthesis of high-efficiency CO 2 reduction electrocatalysts with high C 2 :C 1 , selectivity remains a field of intense interest. Previous studies have shown that the presence of Cu(I) is beneficial for the reduction of CO 2 into C 2 products. However, the stable presence of Cu(I) remains controversial, especially in the negative potential window. Here we report a simple and easily scalable catalyst precursor Cu 2 (OH) 3 Cl/C, which automatically forms in-situ chlorine-doped Cu/Cu 2 O heterointerface during electrocatalysis. The catalyst not only exhibits a Faradaic efficiency of 33.03% but also provides a long-term stability of Cu + , gaining a stable electrolysis of 11 h, with an ethylene/methane ratio over 50. The experimental results and mechanistic studies confirm that the presence of Cl − inhibits the reduction of Cu + , inducing the formation of Cu 0 /Cu + , and reduces the reaction energy of the intermediate ⋆CO dimerization, thereby facilitating the formation of C 2 products. This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO 2 RR and expands a new way to synthesize ethylene industrial products in the future.
研究领域:
材料科学
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电化学
·
催化反应
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Science China-Chemistry
·
2025
·
IF 9.7
Li Ran,Yin Hang,Jing Wen-Kai,Cheng Jia-Lin,Qin Xue-Rong,Lu Tong-Bu,Wang Hong-Juan,Yu Zi-You
As important catalysts for C–C coupling, copper-based materials have great potential for electrocatalytic reduction of CO 2 to C 2+ products. In this work, Cu 2 O catalysts modified with different lanthanide hydroxides were successfully synthesized and used for CO 2 electroreduction. The results showed that compared with Cu 2 O/Gd(OH) 3 and Cu 2 O/Yb(OH) 3 catalysts, Cu 2 O/La(OH) 3 exhibited the highest electrocatalytic performance for CO 2 reduction. This catalyst was able to maintain a high Faraday efficiency for C 2+ products ( \({\rm FE}_{{\rm C}_{2+}}\) ) of about 60% within the current density range of 400–800 mA cm −2 . The highest \({\rm FE}_{{\rm C}_{2+}}\) reached 66% at 600 mA cm −2 and the partial current density for C 2+ products reached a maximum of 488 mA cm −2 . Meanwhile, the catalyst could run stably for 40 h with a remained \({\rm FE}_{{\rm C}_{2+}}\) of about 60%. Multiple characterizations reveal that the introduction of La(OH) 3 promotes the formation of *CO intermediates, and also helps to stabilize the Cu(I) species in Cu 2 O under cathodic potentials, thus facilitating the C–C coupling for C 2+ production. This work provides a new strategy to enhance the C 2+ production via stabilizing Cu(I).
研究领域:
电催化
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二氧化碳还原
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材料化学
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可持续能源
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Erjian Huang,Yueyang Xu,Yachun Ren,Peng Zhang,Yongping Zeng
Faujasite (FAU)-type zeolites are promising adsorbents for the removal of sulfides from fuels, but their micropores are not capable to accommodate the large-sized thiophenic compounds. FAU zeolites (NaX and NaY with the low and high Si:Al ratios, respectively) with hierarchical micro/mesoporous structures were synthesized by sequential acid-base treatment to enhance the adsorption capacity and reduce the limitations of diffusion for the sulfides. To further to improve the desulfurization performance, the hierarchical structure of FAU zeolites containing Cu + were prepared by ion-exchange and methanol vapor-induced reduction methods at a relatively low temperature (473 K). For the large-sized benzothiophene , both the HP-Cu(I)Y and HP-Cu(I)X zeolites with mesopores have a very high adsorption capacity, reaching 51.8 mg S/g and 56.1 mg S/g, respectively. In addition, the results show that HP-Cu(I)X has a higher adsorption capacity than that of some other FAU-type adsorbents reported.
研究领域:
化学工程
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材料科学
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Environmental Science-Water Research & Technology
·
2024
·Vol. 10
·期 8
·1785-1794
·
IF 3.5
Jun Zhang,Shenjun Wang,Yuhao Wu,Jiahai Ma
In advanced oxidation systems, the promoting effect of bicarbonate is relatively overlooked. Bicarbonate, as an inorganic anion widely present in natural waters, is extremely important for water treatment. Therefore, bicarbonate was added to a PDS/Cu2+ system to investigate the degradation mechanisms of organic contaminants. The generation of alkyl radicals in the PDS/Cu2+/HCO3− system was first demonstrated through Electron Paramagnetic Resonance (EPR) testing. This study reveals that the introduced bicarbonate ions undergo transformation into alkyl radicals. The presence of alkyl radicals promotes the cycling of monovalent, divalent, and trivalent copper ions, facilitating the degradation of contaminants. The production of monovalent and trivalent copper ions in the reaction system was confirmed through UV-vis absorption spectroscopy and quenching experiments. Furthermore, the change in the oxidation state of copper ions was further confirmed through EPR testing. These findings not only shed new light on the degradation mechanism of the PDS/Cu2+ system in the presence of bicarbonate but also open up new avenues for the further application of bicarbonate in advanced oxidation processes.
研究领域:
环境科学
·
化学
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Science Advances
·
2026
·Vol. 12
·期 29
·
IF 13.9
Qixing Zhang,Jing Gao,Muchen Li,Ying Yang,Guanlan Chen,Han He,Xingfei Chen,Xiaobing Gu,Yajun Gao,Yongcai He,Bo He,Xixiang Xu,Zhenguo Li,Ying Zhao,Lijun Zhang,Michael Grätzel,Xiaodan Zhang
Solar-driven electrochemical CO 2 reduction to multicarbon (C 2+ ) products presents a promising avenue for artificial photosynthesis, yet remains constrained by high overpotentials and limited conversion efficiency. Here, we developed an alkaline environment-modulated prereduction strategy that capitalizes on the divergent thermodynamic stabilities of precursors, enabling the precise synthesis of iodine-doped copper nanotopologies (Cu-I NTs). Featuring tunable under-coordination defects and stabilized high-energy adsorption sites, the Cu-I NTs achieve an onset potential of only −0.37 V versus the reversible hydrogen electrode for C 2+ formation. Operando Raman measurement and density functional theory calculation reveal that the tailored surface topologies favor Cu-CO rotation adsorption, enabling dynamic reorientation from bridge- to atop-binding configurations, which collectively lowers the barrier for CO-CO coupling. Impressively, powering the electrolyzer by a perovskite/silicon tandem together with a single-junction silicon photovoltaic device, the system delivers a photocurrent of 12.34 mA cm −2 at 2.17 V under standard AM 1.5 illumination, achieving a solar-to-C 2+ conversion efficiency of 8.64%.
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Materials Today Nano
·
2026
·
IF 7.6
Shixiang Rao,Hao Jiang,Zheng Li,Guoqing Wang,Shixing Han,Chunguang Li
Marine biofouling poses serious safety risks to offshore infrastructures and leads to substantial economic losses. Although hydrogels have shown significant promise in marine antifouling applications, developing antifouling hydrogels that simultaneously possess excellent mechanical strength and strong antifouling efficiency remains a major challenge. Herein, a high-performance antifouling hydrogel was constructed by incorporating hollow glass microspheres functionalized with a Cu(I) based metal-organic framework (Cu(I)-MOFs) into a poly(vinyl alcohol)/poly(sulfobetaine methacrylate) (PVA/PSBMA) double-network matrix. The as-developed Cu(I)-MOFs/hydrogel composite integrates excellent antifouling and mechanical properties, achieving protein and algal resistance of 99.8% and 99.9%, respectively, as well as a high antibacterial rate of 99.6%. Importantly, the composite reaches a compressive strength of 5.35 MPa, outperforming many existing antifouling hydrogels, and demonstrates low swelling with reliable performance in seawater. In a 100-day field test in a real marine environment, the fouling coverage of as-prepared hydrogel was as low as 0.12%. This work offers an effective and feasible strategy for preventing marine biofouling and also pioneers a new approach for hydrogel applications. Download: Download high-res image (395KB) Download: Download full-size image
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AICHE JOURNAL
·
2023
·Vol. 69
·期 7
·e18091
·
IF 3.7
Siheng Qian,Jing Hu,Xiaobing Wang,Lifeng Yang,Xian Suo,Zhengbao Wang,Xili Cui,Huabin Xing
Separation and purification of light hydrocarbons have been the critical processes for producing basic chemicals and polymers in petrochemical industry. Adsorbents with high performance are highly demanded for the separation of light hydrocarbons. However, the adsorbents filling in the packed bed when evaluated will inevitably induce reduced performance and increased pressure drop that considerably impede their application. Herein, mixed-matrix fiber adsorbents with anion-pillared hybrid microporous materials (SIFSIX-2-Cu-i) embedded within poly (ether sulfone) (PES) are constructed to enable an energy-efficient propylene/propyne separation. Owing to the sufficient binding sites and abundant channels for selective gas transfer, the fiber adsorbents achieve high C 3 H 4 uptake capacity of 0.963 mmol g −1 in the propylene/propyne (99/1) mixture breakthrough experiments. Moreover, fiber adsorbents exhibit good tolerance toward high gas velocity and show distinctively low pressure drop, which will be advantageous in industrial applications. This work provides a strategy for fabricating high-performance mixed-matrix fiber adsorbents.
研究领域:
化学工程
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材料科学
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CATALYSIS LETTERS
·
2018
·Vol. 148
·期 9
·2709-2718
·
IF 2.911
Liu Zhenzhen,Shen Zhongquan,Zhang Ning,Zhong Wei,Liu Xiaoming
Abstract Homogeneous Cu(I)/NMI/TEMPO catalyst system (TEMPO = 2,2,6,6-tetramethylpiperidine-N-oxyl) has been investigated for its catalysis on the aerobic oxidation of 1-octanol and other alcohols into aldehydes under room temperature. The catalytic species was found to be a Cu(I) centre coordinated by two NMI molecules and other two weakly bound solvent molecules, [Cu(NMI) 2 (Sol) 2 ] + (Sol = solvent). When CuI was used, this species could be [Cu(NMI)I(Sol) 2 ]. Not like being speculated previously, NMI in this system acts solely as a ligand and its role coordinated to the copper centre enhanced the electron density on the metal centre which promoted the O 2 binding in the catalysis. The labile solvent binding to the Cu(I) centre is essential to ensure both oxygen and substrate binding. The catalyst system is suitable for the oxidation of various alcohols using a simple reaction setup and workup. In particular, the system possesses strong oxidizing capability in quantitative conversion of benzylic alcohols regardless of the substituents on the phenyl ring and allylic alcohols into aldehydes. A plausible mechanism was also proposed for the catalysis. Graphical Abstract The aerobic oxidation of primary alcohols at room temperature to corresponding aldehydes was achieved by the catalyst composed by Cu(I) and methyl imidazole (NMI) mediated by TEMPO in acetonitrile. The catalytic species is proposed to be such a Cu(I) complex that two of its four coordinating sites are occupied by a strong ligand(s) and the rest two are weakly bound by solvent molecules.
研究领域:
催化化学
·
有机合成
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WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 14
·791
·
IF 3.5
Yu Lian,Lu Jiarui,Yu Meng,Duan Yajing,Zhang Baofeng,Zhang Xuan,Wang Xiaoyue,Liang Cunzhen
Cu(I) doped Fe 3 O 4 nanoparticles was loaded onto graphene oxide, Cu-Fe 3 O 4 /GO with binary active sites and accelerated Fe(III)/Fe(II) cycle showed higher tetracycline hydrochloride oxidation efficiency than Fe 3 O 4 and Cu-Fe 3 O 4 , the influences of initial H 2 O 2 concentration, reaction pH, catalyst dosage, reaction temperature and radical scavengers on catalytic performance of Cu-Fe 3 O 4 /GO were investigated. The heterogeneous Fenton reaction over Cu-Fe 3 O 4 /GO surface contained Fe(III)/Fe(II) and Cu(II)/Cu(I) active sites, Fe species were the dominant active centers. Cu-Fe 3 O 4 nanoparticles and GO combined via C–O–Fe bond and formed a stable Cu-Fe 3 O 4 /GO conductive structure, which promoted electrons transfer between Cu-Fe 3 O 4 and H 2 O 2 , thus accelerating Fe(III)/Fe(II) and Cu(II)/Cu(I) cycles. GO significantly improved specific surface area, Cu-Fe 3 O 4 nanoparticles dispersibility, and adsorption performance of catalyst. Furthermore, the strong interaction between GO and Cu-Fe 3 O 4 prevented ions from leach, GO captured the soluble Fe(III) which was efficiently reduced to Fe(II) surf by surrounding H 2 O 2 and Cu(I) surf . The degradation efficiency maintained 80.7% after six cycles, the excellent stability can be ascribed to the strong interaction between Cu-Fe 3 O 4 and GO. Reactive oxygen species scavenging results indicated that surface-bound • OH surf played a dominating role, followed by aqueous • OH aq and superoxide radicals (O 2 •− ).
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ACS Biomaterials Science & Engineering
·
2025
·
IF 5.5
Juan Huang,Mingjing Yang,Xingyu Zhou,Jigang Luo,Xiaoxia Yan,Guanghui Lin,Shijie Li,Shihui Liu,Zhuoyue Song,Chunzhi Tang,Nenggui Xu,Tao Liu,Jian Liang
Drug repurposing has received increasing attention in the field of oncology drug development as an alternative strategy to de novo drug synthesis. Disulfiram (DSF) has a long history of clinical application in alcohol withdrawal, and recent studies have revealed that its metabolite diethyldithiocarbamate (DDTC) can be coordinated with copper ions in vivo to form Cu-DDTC complexes with anticancer activity. However, the insufficient in vivo stability of DSF remains a challenge. In this study, the nanomedicine Cu-BTC@DDTC with DDTC-Cu(I) chemical valence and polycrystalline structure was prepared by incorporation of DDTC into the nanosized metal–organic framework (MOF) Cu-BTC. The in vitro cellular evaluation results showed that Cu-BTC@DDTC exhibited high inhibition of tumor cell growth, migration, and invasion. Animal experiments on the xenograft tumor model further demonstrated the excellent antitumor activity and biosafety of Cu-BTC@DDTC, and the antitumor activity was found to be closely related to the regulation of the SLC7A11/GPX4 signaling pathway to induce ferroptosis. This study provides a feasible option for antitumor drug development based on a drug repurposing strategy.
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