JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
·
IF 11.2
Xin Yang,Lijie Zhong,Songxin Ye,Dequan He,Shuxian Yuan,Huixin Li,Yuting Ma,Xiaocheng Mo,Shiyu Gan,Li Niu
Selective electrocatalysis of two-electron oxygen reduction reaction (2e – ORR) has been recognized as a sustainable and on-site process for hydrogen peroxide (H 2 O 2 ) production. Great progress has been achieved for 2e – ORR in alkaline media. However, it is challenged by insufficient activity and selectivity of the catalysts in acidic electrolytes. Herein, we report sulfur-poisoned PtNi/C catalysts (PtNiS x /C) that could regulate ORR from the 4e – to 2e – pathway. The identified PtNiS 0.6 /C offers high activity in terms of onset potential of ∼0.69 V (vs. RHE) and ∼80 % selectivity. The mass activity is also comparable and outperforms representative Pt-based precious and transition-metal-based catalysts. In addition, it is interestingly found that the Faradaic efficiency further increased to 95 % during the long-term electrolysis test due to Ni atom surface migration. The electrochemical production of the H 2 O 2 system was applied to the electro-Fenton process, which has realized the effective degradation of organic pollutants. This work offers a strategy by sulfur poisoning PtNi/C catalyst to realize Pt-based 2e – ORR active catalysts to electrolysis of H 2 O 2 in acidic media.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Xinyi Hu,Hui Xiong,Jiale Dou,Zhao Jiang
It is critical to create the anodic catalysts with high efficiency and economy for direct methanol fuel cells (DMFCs). Here, a series of PtNi/NbN-C catalysts (M=Co, Sn, Ni) are developed using the glycol solvothermal process, to investigate the catalytic effficiency for alkaline methanol oxidation reaction (MOR). Catalytic performance evaluation experiments show that the doped Ni species bring the enhancement effect on Pt/NbN-C for the alkaline MOR. The mass activities of Pt x Ni y /NbN-C show a volcanic trend with the increased Ni contents. PtNi/NbN-C has the highest mass activity (6025.5 mA·mg -1 Pt ) for alkaline MOR, 18.3 times greater than that of the Pt/C commercial catalyst. The LSV, EIS, Tafel, CA and CO stripping results imply PtNi/NbN-C also exhibits the lowest onset potential, charge transfer resistance, fastest kinetics, highest CO tolerance and stability. When the XRD, HRTEM, and XPS analysis are combined, it is discovered that the electronic effect between the Pt, Ni, and NbN species is mostly responsible for the catalytic performance enhancement is mainly depend on the electronic effect among the Pt, Ni and NbN species. The presence of Pt in an electron-deficient state can enhance the conversion of adsorbed methanol and intermediates, evidenced by a direct relationship between the d -band centers and the mass activities for MOR of different catalysts. This study may provide guidance for the development of anodic materials for DMFCs.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
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2024
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IF 6
Xufeng Qin,Weifeng Xu,Jiangnan Hu,Yong Dong,Renbo Ding,Shuheng Huang,Zhendong Zhao,Hong Chang,Xiaokun Wang,Shuai Dong
Glioma, a common primary brain tumor, is highly infiltrative and invasive, often leading to drug resistance and recurrence. Therefore, the development of novel therapeutic agents is urgently needed. Pseudellone C is a novel marine triindole alkaloid. Screening of its antiproliferative activity against 55 cell lines revealed its anti-CNS cancer potential. A total of 42 derivatives of Pseudellone C were designed and synthesized, and their inhibitory activities against two human glioma cell lines (U-87MG and LN-229) were evaluated using the CCK-8 assay. Ten derivatives exhibited potent antiproliferative activity with IC 50 values below 10 μmol, which are 18- to 39- fold more potent than Pseudellone C. Among these, derivative 4o demonstrated favorable blood-brain barrier permeability. Mechanistic studies revealed that 4o induces apoptosis primarily by activating the downstream caspase 3 cascade via the TNF/TNFR pathway. Structure-activity relationship correlations were systematically analyzed, and a pharmacophore model for further rational design was constructed.
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Nature Catalysis
·
2021
·Vol. 4
·期 5
·364-373
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IF 41.813
Cui Yinglu,Wang Yinghui,Tian Wenya,Bu Yifan,Li Tao,Cui Xuexian,Zhu Tong,Li Ruifeng,Wu Bian
Although C–N bonds are ubiquitous in natural products, pharmaceuticals and agrochemicals, biocatalysts forging these bonds with high atom-efficiency and enantioselectivity have been limited to a few select enzymes. In particular, ammonia lyases have emerged as powerful catalysts to access C–N bond formation via hydroamination. However, the use of ammonia lyases is rather restricted due to their narrow synthetic scope. Herein, we report the computational redesign of aspartase, a highly specific ammonia lyase, to yield C–N lyases with cross-compatibility of non-native nucleophiles and electrophiles. A wide range of non-canonical amino acids (ncAAs) are afforded with excellent conversion (up to 99%), regioselectivity >99% and enantioselectivity >99%. The process is scalable under industrially relevant protocols (exemplified in kilogram-scale synthesis) and can be facilely integrated in cascade reactions (demonstrated in the synthesis of β-lactams with N-1 and C-4 substitutions). This versatile and efficient C–N lyase platform supports the preparation of ncAAs and their derivatives, and will present opportunities in synthetic biology.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yangyang Liu,Fengdi Tu,Ziyu Zhang,Zigang Zhao,Pan Guo,Lixiao Shen,Yunlong Zhang,Lei Zhao,Guangjie Shao,Zhenbo Wang
Iron and nitrogen co-doped carbon (Fe/N/C) electrocatalysts have great potential to catalyze the kinetically slow oxygen reduction reaction (ORR). Unfortunately, the ORR performance of existing Fe/N/C catalysts is seriously hindered by the insufficient density and accessibility of the atomic Fe-N x moieties. Herein, the carboxylate (OAc) molecular scissor is proposed to tailor Fe doped zeolitic-imidazolate-framework-8 (ZIF-8) at atomic scale and construct a multi-dimensional concave Fe@NC catalyst structure (Fe@MNC-OAc). This molecular scissoring strategy imparts Fe@MNC-OAc with dense accessible active sites, multidimensional mass transfer pathways, hierarchical porous structure, and entangled carbon nanotubes network. Therefore, the tailored Fe@MNC-OAc electrocatalyst exhibits excellent ORR activity in acidic media with a half-wave potential of 0.838 V, which is comparable to state-of-the-art non-precious metal catalysts. When assembled as cathode catalyst in a H 2 -O 2 proton exchange membrane fuel cell, it delivers a peak power density of 903 mW cm −2 . This work provides a new approach to tailoring the catalyst architecture and improving the accessibility of active sites.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Deqiang Kong,Yueshuai Wang,Yong Yan,Zongge Li,Yue Lu,Ge Chen
Advancing the two-electron (2e - ) oxygen reduction reaction (ORR) in acidic media is pivotal for sustainable, on-demand hydrogen peroxide (H 2 O 2 ) production, but remains challenged by insufficient activity/selectivity at industrially relevant high current densities. We present a breakthrough catalyst design featuring cobalt atomic sites embedded in curved nitrogen-doped carbon layers (c-Co-N-C). This architecture achieves nearly 90 % H 2 O 2 selectivity across a wide potential window, delivering 11.70 mol g⁻¹ h⁻¹ productivity at 300 mA cm −2 with 80 % Faraday efficiency in flow cell tests. Particularly, the catalyst maintains a stable 300 mA cm −2 operation under 1.9 V cell voltage (surpassing prior-art systems by 0.2 V) for 120 h in a PEM electrolyzer, producing pure-phase H 2 O 2 (4.1 wt%). Through integrated experimental and computational analysis, we reveal two complementary enhancement mechanisms: first, the finite element simulations quantify the enhanced interfacial electric field that concentrates protons and dissolved oxygen; then, the density functional theory (DFT) calculations indicate a downshift in Co d -band center optimizes *OOH adsorption while suppressing O-O bond cleavage. This work establishes curvature engineering as a universal design strategy for advanced catalysts through controlled structural modification, opening new pathways for sustainable chemical synthesis.
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Energy Storage Materials
·
2025
·
IF 20.2
Dejun Lu,Yunchao Hao,Zhiqiao Wang,Jun He,Xiaojiang Huang,Yunxiang Shi,Shuai Gao,Huiqing Zhang,Yue Ma,Feng Xu,Yao Yao
Wearable biomedical devices require materials that simultaneously integrate energy storage and sensing, function under extreme conditions, and enable battery self-diagnosis. To address this, we developed a novel ZnCl₂-loaded poly(acrylic acid)-based composite hydrogel (Zn-PAA-C) serving as both a flexible Zn-ion battery electrolyte and a high-performance strain sensor. Engineered with poly(acrylic acid) N-hydroxysuccinimide ester (PAA-NHS), gelatin, and ethylene glycol, Zn-PAA-C exhibits exceptional ionic conductivity, mechanical resilience, and freeze-resistance (down to -80 °C). As a strain sensor, it achieves a broad sensing range (0–180 % strain), reliable operation (1–7 Hz), and rapid response (57 ms). As a battery electrolyte, it uniquely incorporates self-diagnostic capability, enabling real-time monitoring of battery expansion and dendrite formation for enhanced safety and longevity, and supports stable operation over 12,000 charge-discharge cycles. Zn-PAA-C thus transcends traditional gel electrolyte limitations, establishing a new standard for multifunctional materials in wearable biomedical devices capable of robust, continuous health monitoring under extreme conditions.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 21
·2101145
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IF 18.808
Xiaoming Zhou,Yang Liu,Yang Ren,Tiansheng Mu,Xucai Yin,Chunyu Du,Hua Huo,Xinqun Cheng,Pengjian Zuo,Geping Yin
SiO x /C composites with a void-reserving structure are promising anodes for lithium-ion batteries. However, the facile and controllable synthesis of uniformly dispersed SiO x and carbon components, simultaneously incorporating ample voids, still remains a great challenge. Herein, a molecular polymerization strategy is devised to construct SiO x /C hollow particles for lithium-ion batteries. 3-aminopropyltriethoxysilane and dialdehyde molecules are judiciously engineered as silicon and carbon precursors to produce the polymer hollow spheres (PHSs) through a one-step aldimine condensation without any template and additive. A range of PHSs is obtained using terephthalaldehyde, glutaraldehyde, and glyoxal as the crosslinkers, demonstrating the high tunability of the strategy. Importantly, in situ pyrolysis of the PHSs warrants the homogeneous incorporation of SiO x ( < 5 nm) in carbon hollow capsids at a nanocluster scale. The obtained SiO x /C hollow spheres exhibit excellent Li + -ion storage behaviors, including cycling lifespan, coulombic efficiency, and rate performance. The superior performance is attributed to the well-dispersed SiO x nanoclusters in carbon substrate and the hollow structure. This molecular polymerization approach not only enables Si-based hollow composites effective and scalable anode materials but also opens up a new avenue for the controllable synthesis of template-free hollow architectures.
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ACS Nano
·
2022
·
IF 18.027
Yujun Zhang,Shenghua Ye,Min Gao,Yong Li,Xuan Huang,Jun Song,Hong Cai,Qianling Zhang,Junmin Zhang
Heterogenization of homogeneous catalysis through supported single-atom catalysts (SACs) provided a feasible solution to recycling catalysts while keeping its efficiency in chemical synthesis. In this work, Cu SACs anchored on N-doped graphene (Cu SACs/NG) were prepared and first used for C–N coupling reactions. During the preparation, Cu–N–C structures, including Cu–N4 moieties, were formed in a one-step pyrolysis method. As-prepared Cu SACs/NG exhibited excellent catalytic activity toward C–N coupling reactions with a broad scope of substrates and showed outstanding performance of recycling. Compared with Cu nanoparticles (Cu NPs/NG), the advantages of single-atom catalysts were validated via experimental and theoretical calculations. The enhanced performances were attributed to increasing the number of active sites and increasing the intrinsic activity of each active site. This work provides an alternative synthetic strategy for fabricating atomically dispersed SACs and represents a significant advance for coupling reactions.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 16
·6965-6973
·
IF 3.5
Shan Wang,Zhihui Sun,Xuyang Zhao,Kunhua Li,Yafei Wang,Xijing Zhang
Many diseases are due to bacterial infections, which are treated by penicillin. Existing methods for penicillin detection have relatively high requirements for sample storage and processing, personnel professionalism, and instruments. Herein, water-soluble N–C quantum dots (QDs) from wheat straw were synthesized in a green way by using an efficient and simple method. The N–C QDs were modified with an imprinted layer by a gel–sol method. Penicillin selectively quenched the fluorescence emission of N–C QDs@MIP, and a linear relationship was obtained in the concentration range of 1.0 × 10−6–15.2 × 10−6 mol L−1. The reliability of the sensor in real sample analysis was satisfactory with results in the range of 93.6%–100%, and the sensor showed good reproducibility and long-term stability. The study provides a simple strategy to fabricate N–C QDs@MIP with a highly selective recognition ability and opens an avenue to develop highly efficient sensing probes for the detection of antibiotics in biological applications.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yan Sun,Aowen Chen,Jingdao Yang,Kun Zhang,Sikai Wang,Xuerong Xu,Luyue Niu,Yue Jing,Ci Wang,Jing Ren,Jianzhong Zhang
Expanding gain bandwidth into the L-band for erbium-doped fiber amplifiers (EDFAs) is a crucial strategy to overcome limitations in prevalent C-band focused commercial silica-based EDFAs, significantly boosting optical network transmission capacity. Herein, we synthesized Er 3+ -doped broadband near-infrared emission tellurite glasses utilizing the melt quenching process, systematically exploring the impact of ZnCl 2 on the glass structure and optical properties. The 82TeO 2 –3Nb 2 O 5 –15ZnCl 2 –3Er 2 O 3 (TNZ15) glass emerged as a standout candidate for broadband amplifiers around wavelength at 1.55 μm. With escalating ZnCl 2 concentration, a discernible red shift in the emission peak wave lines was observed, accompanied by an expansion of the full width at half maximum (FWHM) from 98 nm to 106 nm. Noteworthy characteristics of all samples included exceptional thermal stability and elevated near-infrared (NIR) transmittance. Application of the Judd-Ofelt (J-O) theory facilitated the calculation of J-O parameter intensity, providing deeper insights into the optical behavior of the materials. Finally, the evaluation of TNZ15 planar optical waveguides, employing the vertical top pumping mode of two 980 nm LEDs, encompassed both the C-band (1530–1565 nm) and the L-band (1565–1625 nm). The results underscore the potential of TNZ15 glass as a promising gain material for broadband optical amplifiers and lasers, offering valuable insights into the development of next-generation optical amplification technologies.
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CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Minghui Jiang,Xiao Liu,Shiyu Li,Yurui Xu,Simai Wang,Lei Lu,Xinxin Li,Xinru Sun,Chunlei Xia,Ziming Wang,Suping Cui
The internal water migration within calcium silicate hydrate (C-S-H) in dry environments is considered to be the primary factor affecting the volume stability of cementitious materials. In this research, the in-situ polymerization product of plant polyphenol tannic acid (TA) was applied to modify C-S-H based on an organic-inorganic composite modification method. The chemical structure, microstructure, composition, dimensional changes and water migration characteristics of modified C-S-H were analyzed. Experimental results showed that TA improved the polymerization degree of siloxane chains in the C-S-H nanostructure, with a maximum improvement of 80.70%, and increased the interlayer spacing in the C-S-H structure, confirming the modification of C-S-H at the nanoscale, exhibited by 29 Si Nuclear Magnetic Resonance (NMR), X-ray diffraction (XRD) and Transmission Electron Microscopy (TEM). This modification by TA optimized the C-S-H nanostructure and microscopic pores, and increased the interlayer and gel pore water content, especially gel pore water increased by 56.53% compared to that of the unmodified C-S-H, revealed by nitrogen adsorption and 1 H LF-NMR. In the dry environment, the blocking and cladding effects of TA on C-S-H effectively inhibited the gel water loss and reduced the drying shrinkage, especially at low TA concentration. This research aims to improve the volume stability of C-S-H by in-situ polymerization product of plant polyphenol, which provides new insights into improving the volume stability of cementitious materials.
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