JOURNAL OF MOLECULAR STRUCTURE
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2017
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IF 1.753
Qi Yao,Chenying Li,Henghui Huang,Hualin Chen,Bailing Liu
A series of carboxyl-terminated hyperbranched oligomer polyester (HBP) with different degree of branching (DB) and number average molar mass ( M ¯ n ) have been prepared. The molecular structure, degree of branching, molecular mass and its distribution of HBP were investigated by FTIR, 1 H NMR, and GPC , respectively. And the coordination number , stability constant and degree of dissociation (α) between HBP and chromium(Ⅲ) were measured via continuous variation method (Job's plot). Experimental results show that the coordination capability between HBP and chromium(Ⅲ) affected by both DB and molecular mass, and the latter plays a decisive role. Moreover HBP outperforms low molecular weight of organic acids (citric acid, acetic acid) and linear polyacrylic acid with similar molecular mass. The coordination number and stability constants of HBP-3 ( M ¯ n = 1713 Da, M ¯ w / M ¯ n (PDI) = 1.11 and DB = 0.72) can reach 4 and 6.55e+008, which demonstrated it can be selected as a good ligand to coordination with chromium(Ⅲ). Therefore HBP can be used as chrome auxiliary in chrome tanning to improve the absorption of chromium.
研究领域:
化学
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材料科学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·
IF 3.7
Yue-Qi Liu,Wen-Hao Pan,Lin-Xia He,Chenglong Han,Tong Lu,Ning-Ning Zhang,Kun Liu
Graphical AlH 3 ·(NMP) x complexes with varying coordination numbers were synthesized. AlH 3 ·(NMP) 1.0 single crystals were isolated from AlH 3 ·(NMP) x mixtures, and successfully elucidated the structure of AlH 3 ·(NMP) 1.0 through single-crystal X-ray diffraction. The coordination number of AlH 3 ·(NMP) x modulates the morphology of Al nanoparticles. AlH 3 ·(NMP) 1.0 exhibited the fastest decomposition rate, yielding highly monodisperse Aluminum nanoparticles (Al NPs) with well-defined shapes and the narrowest size distribution. The controlled chemical synthesis of aluminum nanocrystals (Al NCs) is crucial for their applications in plasmonics, photocatalysis, and optoelectronics. However, there is still a lack of correlation between the precursor of Al hydride N-methylpyrrolidine (AlH 3 ·(NMP) x ) and the Al NC synthesis outcomes. Here, we report the synthesis of AlH 3 ·(NMP) x complexes with different coordination numbers (x from 1.0 to 2.0) and their characterization as precursors regulating the morphology of Al NCs. We isolated AlH 3 ·(NMP) 1.0 single crystals from AlH 3 ·(NMP) x mixtures and successfully elucidated the structure of AlH 3 ·(NMP) 1.0 through single-crystal X-ray diffraction. Importantly, AlH 3 ·(NMP) 1.0 exhibited the fastest decomposition rate, yielding highly monodisperse Al NCs with well-defined shapes and the narrowest size distribution, while higher coordination numbers led to increased dispersity in size and irregular morphologies. Additionally, we observed distinct multipole plasmonic resonances in Al NCs synthesized from lower coordination number precursors, highlighting their superior optical properties. This work establishes a direct correlation between precursor coordination chemistry and Al NC synthesis outcomes, providing a foundation for optimizing nanoparticle production for advanced material applications.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
Progress in Natural Science-Materials International
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2020
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IF 4
D.F. Wu,L.Z. Ouyang,J.M. Huang,J.W. Liu,H. Wang,X.S. Yang,H. Shao,M. Zhu
Hydrolysis of Zr(BH 4 ) 4 ·8NH 3 in deionized water can generate high purity hydrogen at room temperature. However, the sluggish hydrolysis kinetics of Zr(BH 4 ) 4 ·8NH 3 hinders its practical use. To improve its hydrogen generation properties, the effects of magnetic stirring, changing hydrolysis solution and tuning the ammonia coordination number on the hydrolysis properties of Zr(BH 4 ) 4 ·8NH 3 were investigated. Results show that both changing hydrolysis solution and tuning the ammonia coordination number can enhance the hydrolysis kinetics. The hydrolysis kinetics properties of Zr(BH 4 ) 4 ·8NH 3 were significantly improved in MgCl 2 and CoCl 2 solutions. The Zr(BH 4 ) 4 ·xNH 3 (x ≤ 8) samples were synthesized by a ball-milling method with different ammonization time (10, 60 and 180 min). Both the hydrolysis kinetics and hydrogen yield of Zr(BH 4 ) 4 ·xNH 3 (x ≤ 8) were enhanced as the ammonia coordination number (x) decreased. Thus, tuning ammonia coordination number is an effective way to control the hydrolysis properties of Zr(BH 4 ) 4 ·xNH 3 (x ≤ 8).
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Hao Zhang,Xingcong Zhang,Qingdi Sun,Qian He,Hongbing Ji,Xiaohui He
Clarifying the relationship of single metal atom coordination structures and catalytic properties is crucial for the fine-design of highly-efficient catalysts, but systematically manipulating the coordination structure (e.g., coordination numbers (CN) of metal atoms) without changing atomic dispersion is challenging. Herein, we develop a precursor-atomization strategy for the synthesis of single-atom catalysts (SACs) and further precisely tailor Pt-N CN by changing the pyrolysis sequence and atmosphere. It is found that as Pt-N CN decreases (from Pt-N 5 to Pt-N 3 ), the electron density of Pt atoms increases and the energy barrier for H 2 dissociation decreases, thus achieving a ∼550-fold increase in activity of selective hydrogenation of 3-nitrophenylacetylene (reduction of nitro group while maintaining the highly sensitive alkyne group), successfully breaking the selectivity-activity seesaw. Additionally, Pt-N 3 SACs also show remarkably broad applicability for the hydrogenation of nitroarenes (even for iodo-nitrobenzene) due to its unique heterolytic cleavage path of H 2 and preferential adsorption of nitro group.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Chemical Science
·
2025
·
IF 7.4
Yecheng Li,Songjie Meng,Zihong Wang,Hehe Zhang,Xin Zhao,Qingshun Nian,Digen Ruan,Lianfeng Zou,Zhansheng Lu,Xiaodi Ren
Fe single atom catalysts (SACs) with high coordination number have emerged as high-performance catalysts for the conversion of CO2 to CO. However, the influence of alkali cation at the catalyst-electrolyte interface has not yet been understood clearly. Here, we investigate the role of the various alkali metal cations (Na+, K+, Rb+) on catalytic CO2 reduction reaction (CO2RR) behavior on high coordination number Fe SACs (FeN5 and FeN6) obtained from a facile hard template method. We find that larger cations can greatly promote CO2RR and such effects are enhanced with increasing cation concentration. Nevertheless, hydrogen evolution side reaction (HER) on co-existing N heteroatom sites will be worsened. This trade-off highlights the importance of manipulating the reactive sites for SACs. From theoretical simulation and in-situ spectroscopy results, we confirm the functioning mechanism of cations on Fe SACs lies in the enhancement of the adsorption of key intermediates through direct coordination and indirect hydrogen bonding effects. With the rationally designed Fe SACs (FeN5) and the electrolyte condition (1 M KOH), our flow cell test demonstrate a maximum Farady efficiency of CO (FECO) of approximately 100% at 100 mA cm-2. This research provides significant insights for future SACs and electrolyte design.
研究领域:
催化化学
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材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Advanced Optical Materials
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2022
·Vol. 10
·期 18
·2200779
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IF 10.05
Yuning Liang,Wenjie Hu,Xue Yuan,Zaiping Zeng,Baohua Zhu,Yuzong Gu
Metal–organic frameworks (MOFs) are widely explored owing to their excellent nonlinear optical (NLO) properties. However, researchers have mainly focused on designing new structures of MOF crystals to adjust the NLO response while ignoring the influence of the number of metal–ligand coordination bonds on the NLO properties of MOFs. In this study, the influence of the coordination numbers of MOFs on their NLO properties is studied for the first time. Herein, MOFs with different coordination numbers, using trifluoroacetic acid as an auxiliary agent, are synthesized and their NLO properties are tested using the Z-scan technique. The results reveal that the NLO absorption properties of MOFs with high coordination numbers can be effectively modulated from saturable absorption to reverse saturable absorption by increasing the excitation intensity. First-principles calculations show that a change in the coordination numbers leads to a change in the charge transfer from metal to ligand, thereby resulting in different NLO responses. The MOFs with a high coordination number have potential applications in novel optical switches or logic gates. These results provide a reference for the precise adjustment of the NLO properties of MOFs.
研究领域:
材料科学
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光学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2015
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IF 2.337
Binbin Ding,Chaolin Li,Meng Zhang,Fei Ji,Xiaoqing Dong
A power law relation between the filtration coefficients for straining and flux through small pores is reported. This relation can well explain the large penetration depths of particles. However, the normalized effluent concentrations in the experiment and the exponents estimated from the laboratory tests are inconsistent with those from the 2D network model simulation. This study discusses the effects of pore size distribution , capture scheme, and coordination number on the straining-dominant filtration simulation. The findings are compared with experimental data. The sensitivity studies indicate that the two parameters in pore size distribution particularly scale parameter σ , significantly influence the experimental and simulation power law exponent estimation. Three methods are used to estimate the pore size distribution of packing glass granules to obtain a highly accurate pore size distribution. Two capture schemes are applied to 2D pore network models with periodical boundaries and random walk of particles. The normalized effluent concentrations and exponents increase as the coordination number z increases. This trend is more significant in the minimum capture scheme under the same pore size distribution parameters . The simulated normalized effluent concentrations and exponents are consistent with the experimental data under the appropriate simulated conditions. Highly accurate pore size distribution parameters of the porous medium can be inversely determined from laboratory tests with the use of the power law function.
研究领域:
环境工程
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多孔介质传输
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胶体与界面科学
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地下水污染控制
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颗粒迁移
✓ 已验证
DOI
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Junjie Xue,Xuexin You,Fangwei Lu,Haining Zhang,Bo Gao,Chengrui Xin,Fengyu Li,Baimei Tan,Xinhuan Niu,Simin Li,Fan Zhang,Hui Shen
Surface modification represents one of the most effective methods for tailoring the properties of CeO 2 particles in chemical mechanical polishing. Although numerous studies have demonstrated preliminary evidence that ligand structure plays an important role in determining the performance of modified CeO 2 , fundamental insights into the structure-property relationships between ligand coordination number and polishing performance remain lacking in the literature. By comparing the polishing performance of CeO 2 slurries modified by a series of phosphorus ligands with varying numbers of coordination sites-including H 3 PO 4 , aminotrimethylene phosphonic acid (ATMP), and diethylenetriaminepenta(methylenephosphonic acid) (DTPMP)-we demonstrate that ligands with more chelating sites yield superior modification effects. Specifically, optimal performance in terms of suspension stability, material removal rate, and surface quality was observed for slurries modified with DTPMP. Mechanistic investigation through density functional theory calculations reveals that both the coordination strengths and ligand densities on the CeO 2 surface are correlated with their coordination number, which results in distinct performance characteristics of the prepared slurries. This work not only elucidates the fundamental relationships between ligand coordination number and the polishing performance of CeO 2 slurries but also provides a practical strategy for developing high-performance slurries required for chemical mechanical polishing.
研究领域:
材料科学
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表面化学
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纳米材料
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半导体制造
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胶体与界面化学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 21
·7529-7536
·
IF 9.48
Huihuang Chen,Xu Guo,Xiangdong Kong,Yulin Xing,Yan Liu,Bolong Yu,Qun-Xiang Li,Zhigang Geng,Rui Si,Jie Zeng
CO2 electroreduction into valuable products holds great promise for energy supply and environmental remediation but remains a challenge due to the lack of high-performance electrocatalysts. Herein, we developed an efficient strategy to prepare highly active Fe single-atom catalysts (Fe–N5/Fe–N6) by tuning the coordination number of Fe with N towards CO2 electroreduction. The faradaic efficiency of CO for Fe–N5 exceeded 90% ranging from −0.35 to −0.65 V versus the reversible hydrogen electrode (vs. RHE) towards CO2 electroreduction. The turnover frequency of CO for Fe–N5 reached 5006 h−1 at −1.05 V vs. RHE, which was 3.8 times that (1324 h−1) of Fe–N6. Besides, CO was generated at an overpotential as low as 50 mV over Fe–N5, smaller than that (90 mV) over Fe–N6. Density functional theory calculations demonstrated that Fe–N5 facilitated the adsorption and activation of CO2 to form the *COOH intermediate, thus leading to superior selectivity and activity for CO2 electroreduction.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
ACS Nano
·
2019
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IF 13.903
Jinchang Fan,Xiaoqiang Cui,Shansheng Yu,Lin Gu,Qinghua Zhang,Fanqi Meng,Zhangquan Peng,Lipo Ma,Jing-Yuan Ma,Kun Qi,Qiaoliang Bao,Weitao Zheng
Rational control of the components of noble metal alloys is paramount for achieving satisfactory electrocatalytic performances. Though transition metals are commonly used to modify noble metals, many potential elements remain to be explored. Here, we interstitially modulate hydrogen atoms into RhPd nanoparticles to boost the alkaline hydrogen evolution reaction (HER). The obtained stable RhPd-H nanoparticles exhibit pronounced alkaline HER activity with a small overpotential of 36.6 mV at 10 mA cm–2 and a low Tafel slope of 35.3 mV dec–1. The surface electronic state, bond distance, and coordination number of the Rh and Pd atoms are significantly influenced by the presence of interstitial hydrogen atoms. These modifications give RhPd-H nanoparticles a desirable hydrogen adsorption free energy, thus accelerating the hydrogen gas production. We further demonstrate that the interstitial hydrogen atom modulation strategy to improve the HER activity is universal for other Pd-based alloy nanostructures. This work presents a powerful strategy for designing efficient electrocatalysts for the HER and beyond.
研究领域:
材料科学
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电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Biomaterialia
·
2023
·
IF 9.7
Juyang Zhang,Baohong Sun,Ming Zhang,Yutian Su,Wang Xu,Yuhan Sun,Huijun Jiang,Ninglin Zhou,Jian Shen,Fan Wu
Single-atomic nanozymes (SANZs) characterized by atomically dispersed single metal atoms have recently contributed to breakthroughs in biomedicine due to their satisfactory catalytic activity and superior selectivity compared to their nanoscale counterparts. The catalytic performance of SANZs can be improved by modulating their coordination structure. Therefore, adjusting the coordination number of the metal atoms in the active center is a potential method for enhancing the catalytic therapy effect. In this study, we synthesized various atomically dispersed Co nanozymes with different nitrogen coordination numbers for peroxidase (POD)-mimicking single-atomic catalytic antibacterial therapy. Among the polyvinylpyrrolidone modified single-atomic Co nanozymes with nitrogen coordination numbers of 3 (PSACNZs-N 3 -C) and 4 (PSACNZs-N 4 -C), single-atomic Co nanozymes with a coordination number of 2 (PSACNZs-N 2 -C) had the highest POD-like catalytic activity. Kinetic assays and Density functional theory (DFT) calculations indicated that reducing the coordination number can lower the reaction energy barrier of single-atomic Co nanozymes (PSACNZs-N x -C), thereby increasing their catalytic performance. In vitro and in vivo antibacterial assays demonstrated that PSACNZs-N 2 -C had the best antibacterial effect. This study provides proof of concept for enhancing single-atomic catalytic therapy by regulating the coordination number for various biomedical applications, such as tumor therapy and wound disinfection. Statement of significance The use of nanozymes that contain single-atomic catalytic sites has been shown to effectively promote the healing of bacteria-infected wounds by exhibiting peroxidase-like activity. The homogeneous coordination environment of the catalytic site has been associated with high antimicrobial activity , which provides insight into designing new active structures and understanding their mechanisms of action. In this study, we designed a series of cobalt single-atomic nanozymes (PSACNZs-N x -C) with different coordination environments by shearing the Co-N bond and modifying polyvinylpyrrolidone (PVP). The synthesized PSACNZs-N x -C demonstrated enhanced antibacterial activity against both Gram-positive and Gram-negative bacterial strains , and showed good biocompatibility in both in vivo and in vitro experiments.
研究领域:
生物医学工程
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纳米技术
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催化
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抗菌研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 14
·2105787
·
IF 17.521
Jindong Chen,Qingchen Wu,Haotian Tian,Xiaotian Jiang,Feng Xu,Xin Zhao,Zheshuai Lin,Min Luo,Ning Ye
Pnictides are superior infrared (IR) nonlinear optical (NLO) material candidates, but the exploration of NLO pnictides is still tardy due to lack of rational material design strategies. An in-depth understanding structure–performance relationship is urgent for designing novel and eminent pnictide NLO materials. Herein, this work unravels a vital band gap mechanism of pnictides, namely P atom with low coordination numbers (2 CN) will cause the decrease of band gap due to the delocalization of non-bonding electron pairs. Accordingly, a general design paradigm for NLO pnictides, ionicity–covalency–metallicity regulation is proposed for designing wide-band gap NLO pnictides with maintained SHG effect. Driven by this idea, millimeter-level crystals of MgSiP2 are synthesized with a wide band gap (2.34 eV), a strong NLO performance (3.5 x AgGaS 2 ), and a wide IR transparency range (0.53–10.3 µm). This work provides an essential guidance for the future design and synthesis of NLO pnictides, and also opens a new perspective at Zintl chemistry important for other material fields.
研究领域:
材料科学
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非线性光学
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固态化学
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津特尔化学
·
红外材料
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）