MICROCHIMICA ACTA
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2018
·Vol. 185
·期 10
·1-10
·
IF 5.705
Huang Yan-Qin,Yang Li-Na,Wang Yong-Sheng,Xue Jin-Hua,Chen Si-Han
The authors report on a one-pot approach for synthesizing highly fluorescent protamine-stabilized gold nanoclusters. These are shown to be a viable nanoprobe for selective and sensitive fluorometric determination of lead(II) via quenching of fluorescence via Pb(II)-Au(I) interaction. Under optimized conditions, fluorescence measured at excitation/emission peaks of 300/599 nm drops in the 80 nM–15 μM lead(II) concentration range. The detection limit is 24 nM, and relative standard deviations (for n = 11) at concentrations of 0.10, 4.0 and 15 μM are 1.6, 2.5 and 1.9%, respectively. The relative recoveries of added lead(II) in the water samples ranged from 97.9 ± 2.29% to 101.2 ± 1.83%.
Lead(II) ions are found to be able to selectively and sensitively quench the fluorescence of the protamine-gold nanoclusters (PRT-AuNCs). Thereby, an inexpensive, selective and sensitive lead(II) assay was established.
研究领域:
分析化学
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环境科学
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材料科学
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DOI
PubMed
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2022
·Vol. 2022
·期 21
·e202200176
·
IF 2.551
Guanyu Ma,Yun Tang,Leyi Chen,Lubing Qin,Quanli Shen,Likai Wang,Zhenghua Tang
Graphical We report a novel homoleptic alkynyl-protected Au(I)9-Ag(I)9 cluster, which features an intriguing ichthyomorphic assembled core structure. It shows distinct absorbance feature and luminescence properties in solution and in the solid state. Interestingly, it has excellent catalytic performance in both the hydrogen evolution reaction and the reduction of 4-nitrophenol. We report the structure analysis, optical property, and catalytic implications of homoleptic alkynyl-protected Au(I)-Ag(I) nanocluster, namely Au 9 Ag 9 (C≡CAr F ) 18 (abbreviated as Au9 Ag9 hereafter). Single crystal X-ray diffraction analysis disclosed that, the core of Au 9 Ag 9 cluster features intriguing ichthyomorphic assembled structure driven by metallophilic interactions and Au-acetylide linkages. The Au 9 Ag 9 nanocluster is fluorescent in both solution and solid state, and it has much higher quantum yield in solid state. In the electrochemical hydrogen evolution reaction (HER) test, Au 9 Ag 9 nanocluster exhibits a favorable overpotential of 274 mV at 10 mA cm −2 with a Tafel slope of 99 mV dec −1 , which markedly surpass than the [Au(C≡C-Ar F )] f and [Ag(C≡C-Ar F )] f control samples. Furthermore, Au 9 Ag 9 nanocluster shows much higher activity than the other two to catalyze the reduction of 4-nitrophenol.
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高影响因子
Nature Communications
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2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Xiao Kui,Zhang Niyuan,Li Feifei,Hou Dayong,Zhai Xiaoyi,Xu Wanhai,Wang Gelin,Wang Hao,Zhao Liang
Medicinal applications of gold complexes have recently attracted attention due to their innovative antitumor mechanisms. In this work, two hypercoordinated carbon-centered gold clusters PAA4 and PAA5 are quantitatively synthesized by an intramolecular 6- exo - dig cyclization of polymetalated precursors. The on-bench and in vitro experimental studies demonstrate that the characteristic hypercarbon-tetragold(I) multi-center bonding in PAA4 and PAA5 not only guarantees their stability under common physiological conditions, but also facilitates a glutathione (GSH)-triggered prompt and synergetic release of active Au(I) ions in the GSH-overexpressed and acidic microenvironment of human bladder cancer EJ cells. The instantly massive release of coordination unsaturated Au(I) ions causes the efficient inhibition of thioredoxin reductases and then induces a rapid pro-oxidant response, consequently causing the occurrence of accelerated ferroptosis of EJ cells. As a result, these hypercarbon-centered gold(I) cluster prodrugs show high cytotoxicity to bladder cancer cell lines and thus exhibit a significant inhibition effect towards bladder tumors in vivo. Correlation of the synergetic domino dissociation of carbon-polymetal multi-center bonding in metal clusters with the accelerated ferroptosis of cancer cells provides a strategy for metallo-prodrugs and opens a broader prospect for the biological application of metal cluster compounds.
研究领域:
药物化学
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肿瘤学
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无机化学
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药学
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Xinrong Li,Shuliang Chen,Xianzhi Hu,Futing Zi
Thiosulfate as a green and environmentally friendly lixiviant has received great attention in the field of gold extraction. However, the problem of gold ion recovery in thiosulfate gold leaching solution has hindered the large-scale application of this technology. Here, tri-n-butylphosphine (TBUP) was used as a functional monomer to prepare an adsorbent (CTS-TBUP) with abundant pores through the ion crosslinking reaction of chitosan, which was used to recover Au(I) from Au[(S 2 O 3 ) 2 ] 3− solution with high efficiency and large capacity. CTS-TBUP exhibited good potential for industrial applications with a gold loading capacity of 46.34 mg/g. CTS-TBUP exhibited a similar gold recovery performance for all pH ranges from 6 to 11, and the adsorption process of Au(I) on CTS-TBUP was well described by pseudo-second-order kinetics and Langmuir isothermal model. The mechanism by which CTS-TBUP adsorbs gold ions involves ligand exchange between TBUP and Au[(S 2 O 3 ) 2 ] 3− . In addition, Au(I) on CTS-TBUP will be reduced to elemental gold by TBUP in CTS-TBUP. The mechanism of Au(I) adsorption by CTS-TBUP was also confirmed by density functional theory calculations, and confirmed the rationality of forming a complex with a coordination ratio of 2:1 between TBUP and Au(I) at the theoretical level. CTS-TBUP has a good affinity for gold ions in thiosulfate solution, which provides a new idea for the preparation of gold adsorbent.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Molecular Catalysis
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2018
·
IF 0
Xia Chen,Xu Ye,Wen-Yu Liang,Qing Zhou,Giang Vo-Thanh,Ye Liu
The unique amphiphilic Zwitterionic P,O-hybrid ligand ( L1 ) containing phosphino-fragment and −SO 3 − group was synthesized and firstly applied in Au-catalyzed hydration of alkynes. Without the aid of any auxiliary additive such as acid or silver salt, L1 -based Au-catalyst exhibited excellent activity towards hydration of alkynes to yield ketones with 100% selectivity according to Markovnikov’s rule. On the other hand, L1 -based Au-catalyst could be recycled for 4 runs in room temperature ionic liquid of [Bmim]PF 6 without obvious activity loss, and also exhibited wide generality to the hydration of different alkynes.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
ACS Nano
·
2021
·
IF 15.881
Yang Yu,Guojian Yang,Shengrui Zhang,Mo Liu,Shujue Xu,Chunyu Wang,Minjie Li,Sean Xiao-An Zhang
Circular dichroism (CD) chiral sensing is very promising to meet the ever-increasing demands for high-throughput chiral analysis in asymmetric synthesis. However, it is still very challenging to sensitively quantify the composition of enantiomers in a wide concentration range because the existing sensing systems show either linear CD response resultant from stoichiometric chiral transfer or nonlinear CD response resultant from amplified chiral transfer and thus have the drawbacks of low sensitivity and narrow quantification range, respectively. Herein, we propose a sensing system of two-dimensional (2D) Au(I)-thiolate nanosheets. The disordered interligand interactions on the confined surfaces of nanosheets enable the formation of discrete amplified chiral domains around the adsorbed chiral analytes, resulting in a linearly amplified chiral transfer behavior, which provides a solution for highly sensitive and wide-range quantification of enantiomer compositions. Taking (1R, 2R)-(−)- and (1S, 2S)-(+)-1,2-diamino cyclohexanes as example analytes, the concentration and full-range enantiomeric excess (ee) values have been quickly determined by adsorbing them on the surface of Au(I)-MPA (MPA: 3-mercaptopropionic acid) nanosheets in the concentration range of 1.0 × 10–6 to 4.0 × 10–5 M. By engineering the surface functional groups, Au(I)-thiolate nanosheets can be extended to sense other types of analytes, and several polyols with multiple chiral centers have been sensed by boronic acid functionalized nanosheets at the 10–7 M level. The high performances, good extendibility, and one-pot high-yield aqueous synthesis ensure these Au(I)-thiolate nanosheets can be developed as a practical and powerful chiral sensing platform.
研究领域:
分析化学
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材料科学
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纳米技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinrong Li,Shuliang Chen,Zihui Dai,Xianzhi Hu,Futing Zi
The selective recovery of gold ions from gold leaching solutions limits the industrial application of the copper-ammonia (Cu 2+ –NH 3 )-thiosulfate system. Here, the influence of the carbon chain length of organic phosphines on the selective recovery of gold ions was studied, and an extractant (trihexylphosphine, THP) that is suitable for the selective recovery of gold ions from a Cu 2+ –NH 3 -thiosulfate leaching solution was screened. The selectivity of organic phosphines with different carbon chain lengths for gold ions was C 8 = C 6 > C 4 > C 3 > C 2 , and when the number of carbon atoms in a single carbon chain was at least six, the selective recovery of gold ions from the Cu 2+ –NH 3 -thiosulfate solution was realized. THP completely recovered low concentration gold ions (6.73 mg/L) in the Cu 2+ –NH 3 -thiosulfate gold leaching solution regardless of the pH. The mechanism of gold ion extraction into the organic phase mainly involved ligand exchange between THP and [Au(S 2 O 3 ) 2 ] 3− . Job’s method and density functional theory calculations confirmed that the composition ratio of the complex formed by THP and Au was 2:1 at the practical and theoretical levels, respectively. Finally, Multiwfn and VMD were used to visually predict the possible reaction sites in THP. This study provides an exact method for the selective recovery of gold ions from thiosulfate-based gold leaching solutions, which will promote the development of thiosulfate-based gold leaching systems.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2014
·
IF 2.302
Xuezhu Wang,Yongyong Wang,Jing Zhang,Xiaoli Zhao,Ye Liu
A series of ionic Au(I)-complexes ligated by the phosphine-functionalized ionic liquids were synthesized and characterized, which are composed of the Au(I)-complex cation and the counteranion of OTf − , AuCl 4 − , or PF 6 − , respectively. The single crystal X-ray diffraction analyses show that the Au(I)-centered vector in 1A , 1B , 2A , 3A , and 4A all possess the slightly twisted linear geometry, and in each individual the Au(I)-center is coordinated by one chlorine and one imidazolium-based phosphine. The aggregation of 1B in acetone can lead to the formation of the trinuclear Au(I)-complex of 1C due to the aurophilic Au(I)–Au(I) interaction, the electrostatic attraction, and the steric preference. When these ionic Au-complexes were employed as precatalysts for hydration of phenylacetylene in aqueous-methanol media, the reaction proceeded selectively according to Markovnikov's rule with moderate to high yields of acetophenone . The highest activities were achieved over 2A with hydrophobic PF 6 − as the counteranion and the trinuclear 1C under mild conditions (75 °C, 2 h), in conjunction with the additive of proton acid H 2 SO 4 . The ion-pair effect on the catalytic performance of the corresponding Au(I)-complexes, coming from the phosphine-ligated cations and the counteranions, were investigated.
研究领域:
化学
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催化材料科学
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DOI
高影响因子
Small
·
2022
·Vol. 19
·期 11
·2204238
·
IF 15.153
Jing Wang,Jing Zhao,Fang Ma,Liuyun Gong,Yinliang Lu,Weiping Xiao,Hanmin Tang,Chengyi Gao,Yuetong Chen,Jun Ma,Zhan Gao,Jin Yan,Suxia Han
Over half of cancer patients are subjected to radiotherapy, but owing to the deficient amount of reactive oxygen radicals (ROS) and DNA double-strand breaks (DSBs), a fair number of them suffer from radiotherapy resistance and the subsequent short-term survival opportunity. To overcome it, many successes have been achieved in radiosensitizer discovery using physical strategy and/or biological strategy, but significant challenges remain regarding developing clinically translational radiosensitizers. Herein, a peptide-Au(I) infinite coordination supermolecule termed PAICS is developed that combined both physical and biological radiosensitization and possessed pharmaceutical characteristics including adequate circulatory stability, controllable drug release, tumor-prioritized accumulation, and the favorable body eliminability. As expected, monovalent gold ion endowed this supermolecule with high X-ray absorption and the subsequent radiosensitization. Furthermore, a peptide targeting CRM1, is assembled into the supermolecule, which successfully activates p53 and apoptosis pathway, thereby further sensitizing radiotherapy. As a result, PAICS showed superior ability for radiotherapy sensitization in vivo and maintained a favorable safety profile. Thus, the PAICS reported here will offer a feasible solution to simultaneously overcome both the pharmaceutical obstacles of physical and biological radiosensitizers and will enable the development of a class of nanomedicines for tumor radiotherapy sensitization.
研究领域:
癌症研究
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放射肿瘤学
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纳米医学
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药学
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DOI
PubMed
高影响因子
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