ACS Catalysis
·
2021
·
IF 13.084
Yiyang Lin,Kang Liu,Kejun Chen,Yan Xu,Hongmei Li,Junhua Hu,Ying-Rui Lu,Ting-Shan Chan,Xiaoqing Qiu,Junwei Fu,Min Liu
Atomically dispersed FeN4 catalysts have been considered as potential materials to replace Pt-based catalysts for the oxygen reduction reaction (ORR), but they often suffer from sluggish O2 activation kinetics due to the symmetrical charge distribution. Herein, we introduce external N, including pyrrolic-N (PN) and graphitic-N (GN), as an electron acceptor near FeN4 to regulate its charge distribution and improve its ORR activity. Theoretical calculations reveal that introduction of PN evokes much enhanced electron redistribution and local electrical field on the Fe site compared with those observed with GN introduction and the pristine one. Synchrotron X-ray absorption spectroscopy and X-ray photoelectron spectroscopy validate the positive charge accumulation of Fe in the FeN4 site induced by introducing PN. Thus, the obtained FeN4-PN exhibits a great performance for ORR in 0.1 M KOH with a remarkable half-wave potential of 0.91 V versus reversible hydrogen electrode, as well as a Tafel slope of 58 mV decade–1. This work provides a guide to improve the catalytic performances of single-atom catalysts by introducing charge-redistribution sites.
研究领域:
材料科学
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催化化学
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能源科学
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Xinding Yao,Zhenwei Wang,Yue Geng,Hongkun Zhao,Elaheh Rahimpour,William E. Acree,Abolghasem Jouyban
Solubility and relevant thermodynamic properties as well as molecular interactions of clozapine in aqueous systems of protic cosolvent, e.g. isopropanol, and aprotic cosolvents such as acetonitrile, dimethyl sulfoxide (DMSO) and N -methyl-2-pyrrolidinone (NMP) are focus of this paper. The intermolecular interactions and overall charge distribution of clozapine were respectively investigated by using Hirshfeld surface analysis and molecular electrostatic potential surface. All experimentations were executed using a shake-flask approach under p = 101.2 kPa (local pressure) from 278.15 (293.15) to 323.15 (333.15) K. The minimum solubility data of clozapine appeared in neat water for each aqueous system at 278.15 K; and the maximum one, in neat cosolvent at 328.15 K. Correlation of the solubility data (mole fraction) through Jouyban–Acree and MRS models acquired acceptable results with relative average deviations ( RAD ) of no>9.15 %. The solvent descriptors of hydrogen-bonding basicity, solubility parameter and dipolarity-polarizability predominantly controlled the clozapine solubility variation through the quantitative analysis of linear solvation energy relationships in terms of the solubility data at 298.15 K. The extended Hildebrand solubility approach was also employed here to correlate the solubility and study the solvation behavior of solutions. Quantitatively analysis of preferential solvation of clozapine by solvent species in solutions was conducted by the method of inverse Kirkwood–Buff integrals. In the solutions with middle and cosolvent-rich compositions, the parameters of preferential solvation for DMSO, NMP, acetonitrile or isopropanol were positive, which specified that preferential solvation of clozapine was made by co-solvent. In addition, the thermodynamic properties of dissolution of clozapine along with enthalpy–entropy compensation were derived and deeply discussed.
研究领域:
药学
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物理化学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 16
·2313241
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IF 18.5
Cuicui Li,Liang Hu,Xiuyun Ren,Lu Lin,Changzhen Zhan,Qingsong Weng,Xiaoqi Sun,Xiaoliang Yu
Small molecule quinone compounds are attractive cathode materials for rechargeable aqueous zinc-organic batteries (AZOBs) because of their structural diversity and low-cost merits. Among them, nonpolar quinones are dominant given the relatively low solubilities in aqueous electrolytes. However, their poor electronic conductivity and accumulated Coulombic repulsion lead to underutilized active sites and sluggish redox kinetics. Here, polar 2,6-dimethoxy-1,4-benzoquinone ( m -DMBQ) works as an advanced AZOB cathode with unexpectedly superior performance over the nonpolar isomer of 2,5-dimethoxy-1,4-benzoquinone ( p -DMBQ). The asymmetric charge distribution of active centers in the p−π conjugated backbone of m -DMBQ induces reduced bandgap with improved electronic conductivity and redox activity, thus achieving a high specific capacity of 312 mAh g −1 approaching the theoretical limit. Additionally, the lowest unoccupied molecular orbital energy level is lowered for an increased average discharge voltage of 0.88 V. Characterizations and computational studies revealed boosted competitiveness of H + relative to Zn 2+ for significantly enhanced charge transfer kinetics and reversibility. As a result, the as-fabricated AZOB achieves a high energy density of 275 Wh kg −1 based on m -DMBQ along with high-rate capability and long-term cycling stability. This work provides a new molecular engineering strategy through regulating charge distribution symmetry for boosting charge storage in organic cathodes.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
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IF 9.5
Quan Li,Yahui Liu,Yunling Jia,Yanhong Ji,Feng Yan,Jianxin Li,Younas Mohammad,Benqiao He
Constructing a suitable charged surface layer of nanofiltration (NF) membrane is one of the key challenges to achieve efficient Li + /Mg 2+ separation performance with high Mg 2+ /Li + mass ratio ( W Mg2+/Li+ ). Herein, we proposed a facile route, i.e., grafting the short chain amino-rich monomers (SCA, H(NHCH 2 CH 2 ) 1-4 -NH 2 ) instead of conventional amino-rich macro-monomers (ARM), to construct a separation layer with uniform positive charge on the surface of pristine polyamide (PA) NF membrane to achieve effective Li + /Mg 2+ separation. The SCA grafted NF membrane (PA-g-SCA) retained a more uniform distribution of positively charged groups on the PA layer compared with ARM grafted NF membrane. The SCA grafted NF membrane exhibited a high rejection of Mg 2+ and high permeation of Li + at the same time, leading to an extremely high separation factor for Li + /Mg 2+ of 130 even in the W Mg2+/Li+ of 200:1 in the feed, which greatly surpassed those reported. The pure water flux was 1.8 folds than that of the pristine NF membrane due to the hydrophilicity improvement. The results suggested that the distribution uniformity of positive charges could be the key to efficient Li + /Mg 2+ separation of the NF membrane. Our study provided a facile and robust route to design and construct high Li + /Mg 2+ separation performance NF membranes.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Jingrui Jian,Yi Qiao,Fengyi Chen,Changhao Liu,Wangxi Liu,Zhonghua Li,Mingyu Pi,Zhaosheng Li,Zhigang Zou
The substantial discharge of urea-rich wastewater presents a significant threat to the ecological environment. The electrocatalytic urea oxidation reaction (UOR) represents an efficient and environmentally sustainable approach for urea degradation, with its low thermodynamic potential suggesting considerable potential to supplant the oxygen evolution reaction (OER) in energy-efficient hydrogen production from water electrolysis. Although nickel-based catalysts show considerable promise for UOR, the high energy barrier associated with the formation of Ni 3+ remains an obstacle for the reaction. Here, a Ru-doped NiP 2 nanosheet array (NiP 2 -Ru) catalyst was constructed for UOR. The experimental results indicate that Ru doping modulates the local charge distribution of NiP 2 , thereby increasing the oxidation state of Ni. This modification facilitates the formation of highly active Ni 3+ sites, which substantially enhances the UOR activity of NiP 2 . The NiP 2 -Ru catalyst demonstrates exceptional UOR performance, requiring an overpotential of only 0.95 and 0.99 V to achieve a current density of 10 and 100 mA cm −2 with a low Tafel slope of 11.27 mV dec –1 , respectively, in a 1 m KOH solution containing 0.33 m urea, which is comparable to the best reported UOR activity. Furthermore, the catalyst exhibits an excellent stability for over 100 h. This research proposes a viable strategy for the design and synthesis of effective UOR electrocatalysts and advocates further exploration of the application of transition metal phosphides in various environmental and energy-related domains.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Guangyuan Hu,Zhiwei Wang,Changqing Xia,Xinliang Wang,Hongxing He,Zhifeng Nie,Shixing Wang,Weili Li
The recovery of gold from industrial effluents is crucial for environmental conservation, sustainable resource management, and promoting the green development of gold resources. We designed a Zr-based MOF (UKM-78) by incorporating functional organic ligands that resemble amino groups, using MOFs’ inherent sieving effect for ion separation. This novel material exhibited enhanced gold recovery under acidic conditions, with an adsorption capacity three times and an adsorption rate four times higher than those of nonfunctionalized UKM-77. Notably, UKM-78 efficiently captured gold solutions at concentrations as low as 1 ppm and achieved an adsorption rate exceeding 90%, owing to the electrostatic interactions and coordination between its functionalized groups and the synergistic effect of its porous structure. Despite multiple regeneration cycles, UKM-78 retains 99.4% of its adsorption capacity. X-ray photoelectron spectroscopy (XPS), kinetic studies, and thermodynamics collectively demonstrated that Au(III) binding on UKM-78 involved cooperative electrostatic interactions and chemical adsorption through coordination. This study highlights the potential of MOFs for efficient and sustainable recovery of gold from complex waste streams.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
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IF 5.4
Tong Gao,Shu-Yu Zhou,Pengpeng Dai,Jidong Song,Junhong Liao,Yuxuan Sun,Chenglong Yu,Shi-Xi Zhao,Guozhong Cao
Single-crystal Ni-rich ternary cathode materials (811), with their comprehensive advantage of high energy density and low manufacturing cost, have been considered the most promising materials for Li-ion batteries. Due to strong O-p/TM-d covalent hybridization, the complete oxidation of Ni ions during electrochemical cycling is often accompanied by inevitable oxygen loss, resulting in an irreversible surface phase transition, accumulated lattice stress, and poor thermal stability. Considering the fact that introducing heteroatoms into traditional doping systems can alter the electron density distribution around coordinated oxygen, compositionally complex systems based on high-entropy doping may have a more significant effect on stabilizing lattice oxygen. Herein, the high-entropy doping strategy was applied to design and synthesize single-crystal NCM811 cathodes (HE811) through the molten salt method. Compared to 811, HE811 cathodes show an excellent initial Coulombic efficiency of 90.74% at 0.2C and deliver a higher capacity retention of 80.79% after 300 cycles at 1C between 2.8 and 4.3 V. Owing to high-entropy doping, the oxygen electron densities around multidopants are increased, inhibiting the excessive oxidation of lattice oxygen and improving the stability of TMO6 coordination structures. This work could provide insights into the high-entropy doping effects in modulating oxygen charge distribution to design high-energy-density Ni-rich ternary cathode materials with long-term cycling.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2019
·Vol. 46
·期 1
·509-520
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IF 2.064
Tang Chang-cun,Fang Yan-fen,Cao Xin-qiang,Tian Hai-lin,Huang Ying-ping
In this paper, bismuth oxybromide (BiOBr) photocatalysts were synthesized in the presence of tetrabutylammonium bromide (TBAB) at the different volume fractions of ethanol/water and named as BiOBr 0 , BiOBr 20 , BiOBr 50 , BiOBr 80 and BiOBr 100 , respectively. The samples were characterized and applied to the degradation of Rhodamine B (RhB) under visible-light irradiation ( λ ≥ 420 nm). The results indicated that both TBAB and ethanol significantly affected the crystal phase, morphology and surface charge distribution of BiOBr. The exposed (110) faces of BiOBr with Bi 3+ sites contributed to its photocatalytic activity via the enhanced separation of electrons and photogenerated holes as well as the better photo-stability. BiOBr 50 showed the optimal activity for the photodegradation of RhB. Superoxide radical (O ·− 2 ) as the dominant active species was responsible for the degradation of RhB.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Minhua Ai,Lun Pan,Ying Chen,Chengxiang Shi,Zhen-Feng Huang,Xiangwen Zhang,Ji-Jun Zou
The periodical distribution of N and C atoms in the carbon nitride skeleton results in intrinsically insufficient light absorption and serious carrier recombination. Herein, an efficient two-step cystine-mediated strategy was developed to alter the structure symmetry of C 3 N 4 via the introduction of alkyl groups and nitrogen vacancies. The experimental analysis and theoretical calculation confirm that the formation of alkyl groups and nitrogen vacancies can modulate band structure and activate n-π* electron transition. Especially, the charge density in CN-25CYS is redistributed with spatial separation of oxidation and reduction sites, suppressing photogenerated charge recombination effectively. Therefore, the distorted carbon nitride (CN-25CYS) exhibits 9.6-times and 15.6-times higher photoreaction rates in hydrogen production and RhB degradation than the pristine one (CN-0CYS), respectively.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Xiaodong Huang,Zhen Zhang,Xiang-Yu Kong,Yue Sun,Congcong Zhu,Pei Liu,Jinhui Pang,Lei Jiang,Liping Wen
Nature is the source of human being's creativity and always inspires people to break through the existing bottleneck of science and technology. Electric eel (Electrophorus electricus) relying on ion channel in electrocyte can convert salinity gradient energy to electricity power with potentials of ~600 V to stun prey and ward off predators. Inspired by biological ion channels, artificial nanochannels have been extensively explored to mimic the control of ion flow in nanosize confinement space and apply in salinity gradient power generation. In this paper, polyether sulfone/sulfonated polyether sulfone (PES/SPES) membranes with large amount of nanochannels are constructed by using phase separation method to be applied in the salinity gradient power generation field. The content of SPES, the concentration of casting solution , and the thickness of prefabricated membrane were taken into account to control the structural and surface charge distribution of membrane. The prepared serials PES/SPES membrane with nanopore structure display much proper cation selectivity, excellent ion conductivity and output power density (reach up to 2.48 W/m 2 ) for salinity gradient power generation. In addition, the proposed membrane with low cost and easy casting process shows great potential for the practical application in salinity gradient power generation.
研究领域:
材料科学
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能源技术
·
仿生学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2023
·
IF 4
Zong-Bao Yu,Zhuozhuo Song,Peng Zheng,Jie Sun,Zhanxu Yang
Transition metal sulfides (TM sulfides) has long been regarded as highly promising materials for catalyzing oxygen evolution reaction (OER). The function of TM sulfides in OER occurs on TM oxyhydroxide and SO 4 2− , which are formed through surface reconstruction under certain potentials. It is worth noting that the impact of SO 4 2− on the local charge distribution among atoms, a crucial determinant of OER performance, has been insufficiently studied. This study aims to investigate the role of SO 4 2− in mediating the partial redistribution of charges among Co, Ni and O atoms on a precatalyst Co 9 S 8 /C–Ni(OH) 2 electrode. The electrode undergoes self-reconstruction to form a CoOOH/SO 4 2− /NiOOH structure on its surface that is active for the OER. The results demonstrate that SO 4 2− facilitates the local charge redistribution of active atoms, leading to optimized adsorption energy of OER intermediates and increased redox center of the material. Furthermore, SO 4 2− serves as an electron mediator in the OER process under varying applied voltages. Consequently, CoOOH/SO 4 2− /NiOOH achieves a Tafel slope of 56 mV dec −1 , an overpotential of 250 mV, and maintains a high stability for over 100 h at a current density of 20 mA cm −2 . Overall, this research provides valuable insights into catalytic reaction mechanisms and the design of efficient composite catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Wenyan Ji,Yuping Li,Feng Duan,Lulu Liu,Renqiang Cao,Jingya Yin,He Sun,Jianquan Luo,Hongbin Cao
Nanofiltration membranes are essential for lithium recovery from brine, but their selectivity declines under high-salt conditions due to electrostatic shielding and fouling. We introduce a novel strategy to enhance membrane performance by enhancing positive charge density on the membrane surface while creating negative charge microdomains within the membrane. Specifically, we functionalized a polyethyleneimine-based membrane with 1,4-butanesultone through a ring-opening reaction, which balanced ion-membrane affinity and optimized the transport kinetics of water and ions. The resulting membrane exhibited a significant enhancement in permeance up to 11.2 L m −2 h −1 bar −1 and selectivity for Mg 2+ /Li + up to 51. Notably, it maintained over 96.21 % MgCl 2 rejection across a wide salt concentration range of 1–20 g L −1 , outperforming the results reported in literature. The comprehensive testing and mechanistic study indicate that this improved performance is due to the synergy of Donnan effect and ion-attraction, facilitated by the designed charge distribution. A two-stage nanofiltration process employing this membrane reduced the Mg 2+ /Li + ratio in brine samples from 43 to 0.25, highlighting its practical application potential. This work introduces a new paradigm for the design of highly selective membranes.
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
危险品化学品经营许可证（带存储）