Matter
·
2025
·
IF 17.5
Bohan Li,Yongsheng Sun,Yuzhen Wang,Jiance Jin,Kai Han,Yan Xu,Zhiguo Xia
Highly transparent and large-area scintillator film is highly desirable for next-generation X-ray imaging and detection. Herein, we develop a rapid and in situ synthesis strategy to fabricate polymer scintillator film composed of (C 14 H 15 P) 4 Cu 4 I 4 glassy cluster gel (M1-GCG). The large-area M1-GCG film of 20 × 12 cm was obtained by in situ UV photopolymerization within 30 s, showing ∼90% transmittance in the broad spectral region of 400–1,000 nm, in which Cu(I) iodide clusters coordinated by phosphine ligands are generated as a glassy form in the polymer network structure and uniformly distributed under supramolecular interactions, as the polymer monomer is polymerized and cross-linked under ultraviolet light. We develop a brand-new chemical synthesis route toward polymer-based composite scintillator film, and the M1-GCG film with high transparency and scintillation properties, as well as high-resolution X-ray imaging ability, shows extraordinary potential for large-area medical imaging and industrial non-destructive detection.
研究领域:
材料科学
·
核工程
·
光学材料
·
辐射探测
·
高分子化学
·
医学成像技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Cheng-Feng Liang,Song-Hai Wu,Yu-Le Wang,Zhi Xu,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,Xu Han
Thiosulfate (S 2 O 3 2− ) is an important ligand to complex metal cations, however, the reactivity of metal-thiosulfate complexes has barely been mentioned. In this study, the reactivity of the Cu(II)–S 2 O 3 2− system in the reduction of Cr(VI) was investigated. Kinetic results show that the reduction rates of Cr(VI) decrease with increasing pH values from 3.0 to 5.0, and 94.3% and 97.5% of 10 mg L −1 Cr(VI) was rapidly reduced within 1 min at pH 3.0 and within 30 min at pH 5.0, respectively at the molar ratio of Cu(II):S 2 O 3 2− of 0.05. We rule out the contributions of S species of tetrathionate (S 4 O 6 2− ) and sulfite (SO 3 2− ) to Cr(VI) reduction and point out that the produced Cu(I) in the Cu(II)–S 2 O 3 2− system is the key reductant that mediates the reduction of Cr(VI). We suggest that complexation between Cu(II) and S 2 O 3 2− with the formation of Cu II (S 2 O 3 ) 2 2− is the pre-requisite for the formation of Cu I (S 2 O 3 ) n 1−2n , which plays an important role in Cr(VI) reduction, accompanied by the re-oxidation of Cu(I) to Cu(II) by Cr(VI), achieving the rapid redox cycling of Cu(II)–Cu(I)–Cu(II). Such a redox cycle also mediates the denitrification process of NO 2 − to NH 3 /NH 4 + under weakly acidic conditions. This study enriches our understanding on the reducing reactivity of the Cu(II)–S 2 O 3 2− system and the importance of the Cu(II)–Cu(I)–Cu(II) redox cycle towards environmental oxidizing contaminants.
研究领域:
环境化学
·
配位化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Huiwang Dai,Jingyi Zhu,Fanxu Meng,Daohui Lin,Wenjun Zhou,Dingjiang Chen,Ming Zhang,Qingqing Wang
In this study, Cu hybridization coupling oxygen defect engineering was adopted to synthesis of CuNiFe layered double oxides (CuNiFe-LDOs) in peroxymonosulfate (PMS) activation for degradation of methyl 4-hydroxybenzoate. The morphology and crystal structure of CuNiFe-LDOs was characterized in detail, which exhibited regular layered-structure at a Cu:Ni doping ratio of 1:1 and annealing temperature of 400 °C, and presented the crystal of Cu x O@Fe 3 O 4 –NiO. Besides, the X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) results demonstrated that abundant oxygen vacancies (OVs) and low oxidation state Cu species were composed in CuNiFe-LDOs400. The Cu 1·5 Ni 1·5 Fe 1 -LDOs400/PMS system showed excellent catalytic performance toward the degradation of butyl 4-hydroxybenzoate (BuP), and resistant to the effect of pH value and background inorganic anions. Based on quenching experiments and EPR measurements, singlet oxygen ( 1 O 2 ) was identified as the dominant active species during the heterogeneous catalytic process, which was generated by the synergistic interaction between OVs-Cu(I) site and PMS . In this process, the electron-drawing property of OVs promoted the adsorption of PMS molecule on Cu(I) site, followed by the accumulation of electron and cleavage of O–O bond to generate intermediate oxygen radical species, which donated one electron to eventually generate singlet oxygen.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy & Environmental Science
·
2016
·Vol. 9
·期 12
·3736-3745
·
IF 25.427
Haihua Wu,Haobo Li,Xinfei Zhao,Qingfei Liu,Jing Wang,Jianping Xiao,Songhai Xie,Rui Si,Fan Yang,Shu Miao,Xiaoguang Guo,Guoxiong Wang,Xinhe Bao
A coordinatively unsaturated copper–nitrogen architecture in copper metalloenzymes is essential for its capability to catalyze the oxygen reduction reaction (ORR). However, the stabilization of analogous active sites in realistic catalysts remains a key challenge. Herein, we report a facile route to synthesize highly doped and exposed copper(I)–nitrogen (Cu(I)–N) active sites within graphene (Cu–N©C) by pyrolysis of coordinatively saturated copper phthalocyanine, which is inert for the ORR, together with dicyandiamide. Cu(I)–N is identified as the active site for catalyzing the ORR by combining physicochemical and electrochemical studies, as well as density function theory calculations. The graphene matrix could stabilize the high density of Cu(I)–N active sites with a copper loading higher than 8.5 wt%, while acting as the electron-conducting path. The ORR activity increases with the specific surface area of the Cu–N©C catalysts due to more exposed Cu(I)–N active sites. The optimum Cu–N©C catalyst demonstrates a high ORR activity and stability, as well as an excellent performance and stability in zinc–air batteries with ultralow catalyst loading.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2021
·
IF 1.751
Yan Zhao,Xianying Duan,Guangguang Zhang,Meilin Wei
Two proton-conductive and luminescent organic-inorganic hybrid materials, {[Cu(II)(bhmbpy)(H2O)(Cl)0.5(CH3CN)]2[PW(VI)10W(V)2O39]}·4H2O(1) and {H2[Cu(I)(bhmbpy)2(Cl)Cu(I)(bhmbpy)2][PW12O40]}·7H2O (2) (where bhmbpy is bis(hydroxymethyl)-2,2′-bipyridine), were synthesized at room temperature. The two products were characterized by infrared spectroscopy, X-ray single-crystal diffraction, X-ray powder diffraction, elemental and thermogravimetric analyses. The proton conductivities and luminescence of 1 and 2 were studied by using alternating-current impedance spectroscopy and luminescence spectroscopy, respectively. X-ray diffraction analysis revealed that 1 includes a decorated polyanion chain {[Cu(II)(bhmbpy)(H2O)(Cl)0.5(CH3CN)]2[PW(VI)10W(V)2O39]}n and forms a three-dimensional network structure depending on short Cl…Cl contacts and hydrogen-bonding interactions. X-ray diffraction analysis revealed that 2 includes a butterfly-like bi-nuclear copper cluster unit with a Cl-bridge, [Cu(I)(bhmbpy)2(Cl)Cu(I)(bhmbpy)2]+, and forms a three-dimensional network structure depending on hydrogen-bonding interactions. [PW12O40]3– anions fill in the network based on hydrogen-bonding and electrostatic interactions. In them, the bhmbpy acts as a bidentate nitrogen donor ligand in the chelating fashion to coordinate with the Cu(II) center in 1 and the Cu(I) center in 2. The bhmbpy in 2 successfully constrains the Cu(I) within a rigid environment in a tetragonal-pyramidal geometry. The two compounds exhibit good proton conductivity (10−4 S·cm−1) at 100 °C in the relative humidity range 35–98%. Their luminescence behaviors in the solid state at room temperature have also been investigated. Upon excitation at 384 nm, 1 exhibits three emission peaks centered at 439, 507 and 566 nm. When excited at 364 nm, 2 displays three emission peaks centered at 443, 501 and 553 nm.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 14
·4045-4053
·
IF 7
Zhaoguo Hong,Xin You,Jingjing Zhong,Di Yao,He-Dong Bian,Shulin Zhao,Liangliang Zhang,Hong Liang,Fu-Ping Huang
Chemodynamic therapy (CDT), in which highly toxic hydroxyl radicals (˙OH) could be triggered by a Fenton or Fenton-like reaction to kill cancer cells, has emerged recently. Compared to traditional CDT nanomaterials, herein, an atomically-precise biotinylated Cu(I/II) complex [CuICuIICl2(VBio)]·CH3OH (VBio = deprotonated O-vanillin biotinylhydrazone), denoted VBio-CuICuII, was rationally designed and synthesized successfully. This targeted Fenton-like agent, VBio-CuICuII, is constructed from a hydroxyl radical-producible CuI ion, a CuII center as a GSH depletor for an augmented CDT effect, and a biotin moiety as a cancer-targeting unit. Owing to the obvious cell selectivity discrepancy of biotin towards normal and cancerous cells, VBio-CuICuII was able to preferentially accumulate in tumor cells. Meanwhile, the CuI metal center could be used as a Fenton-like agent to generate ˙OH. Furthermore, the CuII in VBio-CuICuII was available for successive ˙OH production via a CuI/CuII-circulation strategy under a GSH-rich tumor site, thereby improving catalytic efficiency. More importantly, in vivo results further demonstrate that VBio-CuICuII could significantly inhibit tumor growth without obvious damage toward major organs. Therefore, this multiple-identity Fenton-like agent could provide an appreciable reference value for the design of atomically precise CDT agents.
研究领域:
癌症治疗
·
无机化学
·
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Cheng Chen,Li Liu,Jing Guo,Lixiang Zhou,Yeqing Lan
Sulfur-doped copper-cobalt bimetallic oxides (S-CuYO) with abundant Cu(I) were successfully synthesized by a co-precipitation method and were for the first time utilized to activate peroxymonosulfate (PMS) for the degradation of chloramphenicol (CAP). For comparison purposes, sulfur-doped monometallic oxides (S-CuO and S-CoO) and non-doped copper-cobalt bimetallic oxide (CuCoO-1) were also prepared via the same processes. The results demonstrated that S-CuCoO had the highest catalytic activity among the catalysts. The sulfur-doped catalyst significantly improved the catalytic performance and stability. More than 98% of CAP (20 mg/L) was removed within 15 min at the initial pH = 5. The superior catalytic activity of S-CuCoO mainly resulted from the synergy of Cu(I) and Co(II). The presence of Cu(I) improved the conversion of Co(III) to Co(II), which maintained the high catalytic performance of S-CuCoO. In addition, the produced Cu(II) was further converted to Cu(I) by lattice oxygen (O 2− ), ensuring an adequate supply of Cu(I) in the catalyst. Radical quenching experiments revealed that both the SO 4 − and OH radicals were generated by the interaction of S-CuCoO with PMS, thereby contributing to the efficient degradation of CAP and the OH radicals played a larger role. The main intermediates of the CAP degradation were identified by high-performance liquid chromatography–mass spectrometry (HPLC-MS/MS). Theoretical calculations of the frontier electron densities (FEDs) were performed to determine the possible degradation pathways of CAP.
研究领域:
环境化学
·
材料科学
·
催化
·
水处理
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Hui Zhang,Qiang Fu,Hongyun Qin,Xia Chen,Qicheng Zhang,Zixu Dong,Haoyuan Li,Shoudong Wang,Ming Wang
Hydrogen recovery from ammonia purge gas is a desirable method to relieve the pressure of increasing demand for hydrogen. Metal-organic frameworks (MOFs) are promising adsorbents for the separation of the H 2 –N 2 mixture. However, the separation of the H 2 –N 2 mixture using MOFs remains challenging due to the lack of adsorptive mechanism. Herein, the adsorption mechanism of the H 2 –N 2 mixture in SIFSIX-2-Cu-i has been systematically investigated with the method of a combination of excess adsorption experiments, molecular simulations , and DFT calculations. In the Grand Canonical Monte Carlo (GCMC) simulations, the polarizable force field was first applied to the adsorption of pure H 2 or N 2 and H 2 –N 2 mixture in SIFSIX-2-Cu-i. Ab Initio Molecular Dynamics (AIMD) was performed to investigate the distribution of the guest molecules in the pores of SIFSIX-2-Cu-i. Finally, Density functional theory (DFT) calculations were performed to predict the transfer of charge between MOF and guest molecules. Results revealed two binding sites of H 2 or N 2 in SIFSIX-2-Cu-i. A relatively high thermodynamic adsorption selectivity for N 2 over H 2 has been observed in SIFSIX-2-Cu-i. Furthermore, SIFSIX-2-Cu-i also exhibits a greater affinity with N 2 than with H 2 , which is probably because of the stronger induction interactions between F2 atoms and N 2 molecules. These findings are of significance to guide the design of the new highly selective adsorbents for the separation of H 2 /N 2 .
研究领域:
化学工程
·
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 10
·e2206619120
·
IF 11.1
Wencui Li,Zhi Li,Hang Zhang,Pengxiao Liu,Zean Xie,Weiyu Song,Baijun Liu,Zhen Zhao
Selective oxidation of methane to organic oxygenates over metal–organic frameworks (MOFs) catalysts at low temperature is a challenging topic in the field of C1 chemistry because of the inferior stability of MOFs. Modifying the surface of Cu-BTC via hydrophobic polydimethylsiloxane (PDMS) at 235 °C under vacuum not only can dramatically improve its catalytic cycle stability in a liquid phase but also generate coordinatively unsaturated Cu(I) sites, which significantly enhances the catalytic activity of Cu-BTC catalyst. The results of spectroscopy characterizations and theoretical calculation proved that the coordinatively unsaturated Cu(I) sites made H2O2 dissociative into •OH, which formed Cu(II)-O active species by combining with coordinatively unsaturated Cu(I) sites for activating the C−H bond of methane. The high productivity of C1 oxygenates (CH3OH and CH3OOH) of 10.67 mmol gcat.−1h−1 with super high selectivity of 99.6% to C1 oxygenates was achieved over Cu-BTC-P-235 catalyst, and the catalyst possessed excellent reusability.
研究领域:
催化
·
化学工程
·
材料科学
·
无机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wen-Jian Yang,Li-Hui Yang,Han-Jun Peng,Si-Hao Lv,Hafiz Muhammad Adeel Sharif,Wei Sun,Wei Li,Cao Yang,Hui Lin
Electroreduction removal of nitrate (NO 3 – -N) is considered as a promising approach to solve its adverse effects on environment and human health, where efficient and cheap catalysts are required. Perovskite-based catalysts showed a versatile catalytic ability for wide range of redox reactions, but seldom applied for NO 3 – -N reduction. Herein, four perovskite oxide cathodes, LaMO 3-δ (M = Fe, Co, Ni and Cu) were prepared and used for the reduction of NO 3 – -N. The Ruddlesden-Popper (RP) type La 2 CuO 4 exhibited the best NO 3 – -N catalytic activity among the four perovskite oxide cathodes, with a removal rate of 11.7 × 10 -3 min −1 . The high selectivity of NH 4 + -N (82.4 ± 2.2%) indicated that NH 4 + -N was the main final product for NO 3 – -N electroreduction at La 2 CuO 4 cathode, but 100% of N 2 selectivity could be obtained with addition of 1000 and 1500 mg/L Cl - as the electro-assisted chlorination process. The mechanism of NO 3 – -N electroreduction occurred by both electron- and H*-mediated pathway, and the oxygen vacancies and redox cycle of Cu(I)-Cu(II)-Cu(I) were proposed as the accommodation sties and direct electron sources for NO 3 – -N reduction. Generally, this study opens a novel avenue for the development of earth-abundant, cost-effective catalyst with effective NO 3 – -N electroreduction.
研究领域:
环境科学
·
催化
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Photonics Research
·
2021
·Vol. 2
·期 9
·2100066
·
IF 0
Jia-Li Yao,Zi-Xu Zhang,Xiao-Qi Sun,Tong Chang,Jing-Fu Guo,Ke-Ke Huang,Hai-Bo Zeng,Da-Yang Wang,Wen-Sheng Yang,Ruo-Sheng Zeng,Xiao-Ming Li,Ren-Guo Xie
Radioluminescence materials (scintillators) are widely investigated because of their potential application in many fields, such as medical imaging, security-related techniques, and nondestructive inspection. However, the fabrication of scintillator materials with simultaneously fast response time, high absorption coefficient, and high light yield, as well as low toxicity is still a challenge. Herein, the synthesis of Cu(I)-doped Cs 2 AgI 3 single crystals (SCs) with a 1D crystal structure is presented. A bright blue-green photoluminescence (PL) is observed after incorporating Cu + into the Cs 2 AgI 3 SCs under UV irradiation at room temperature. The PL quantum yield of the doped samples can reach up to 73% at a Cu + concentration of 0.66%. Experimental and theoretical studies show that the blue-green emission may originate from self-trapped excitons, which is further verified by photophysical results from control experiments on pure Cs 2 AgI 3 SCs. Upon X-ray excitation, Cu-doped SCs exhibit fast scintillation decay time (288 ns), high light yield (27 000 photons per MeV), and high absorption coefficient compared with the commercial product (CsI: Tl). These results suggest that Cu-doped Cs 2 AgI 3 is an ideal scintillator, which will be a promising candidate for potential application in dynamic real-time imaging and radiation detection.
研究领域:
材料科学
·
医学成像
·
辐射检测
✓ 已验证
产品关联
DOI
Small
·
2024
·
IF 13
Yi-Ran Du,Xiao-Qiang Li,Xian-Xia Yang,Guo-Yi Duan,Yong-Mei Chen,Bao-Hua Xu
In this study, the copper-nickel (Cu–Ni) bimetallic electrocatalysts for electrochemical CO 2 reduction reaction(CO 2 RR) are fabricated by taking the finely designed poly(ionic liquids) (PIL) containing abundant Salen and imidazolium chelating sites as the surficial layer, wherein Cu–Ni, PIL–Cu and PIL–Ni interaction can be readily regulated by different synthetic scheme. As a proof of concept, Cu@Salen-PIL@Ni(NO 3 ) 2 and Cu@Salen-PIL(Ni) hybrids differ significantly in the types and distribution of Ni species and Cu species at the surface, thereby delivering distinct Cu–Ni cooperation fashion for the CO 2 RR. Remarkably, Cu@Salen-PIL@Ni(NO 3 ) 2 provides a C2+ faradaic efficiency (FE C2+ ) of 80.9% with partial current density ( j C 2+ ) of 262.9 mA cm −2 at −0.80 V (versus reversible hydrogen electrode, RHE) in 1 m KOH in a flow cell, while Cu@Salen-PIL(Ni) delivers the optimal FE C2+ of 63.8% at j C2+ of 146.7 mA cm −2 at −0.78 V. Mechanistic studies indicates that the presence of Cu–Ni interfaces in Cu@Salen-PIL@Ni(NO 3 ) 2 accounts for the preserve of high-valence Cu(I) species under CO 2 RR conditions. It results in a high activity of both CO 2 -to-CO conversion and C–C coupling while inhibition of the competitive HER.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）