MACROMOLECULAR RAPID COMMUNICATIONS
·
2010
·Vol. 31
·期 21
·1886-1891
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IF 4.263
Wei Xiong,Hanfu Wang,Yanchun Han
Novel dendritic triblock co-oligomer (14G2A3) consisting of ester dendrons and aniline oligomer was synthesized and found to self-assemble into fibrils in THF. Studies reveal that the formation of the fibrils originates from both of the amphiphilic interactions between the ester dendrons and oligoaniline, as well as the intermolecular π-π stacking among oligoanilines. The shape effect of dendrons on molecular packing was comparatively analyzed with packing parameter against its linear analogous compound. At the same time, the driving forces that dominate the final aggregating state of the block oligomer were separately investigated using the bulky-group protecting method, which allows release of the intermolecular π-π stacking of oligoaniline in a controlled manner. Results show that both the introduction of dendrons and the intermolecular π-π stacking will increase the packing parameter of the block oligomer and, consequently, cause the self-assembly morphology to evolve step by step from micelles to vesicles and finally to fibrils. The fibrils can form complexes with SWNTs to increase solubility in THF. The effective fluorescence quenching accompanied also opens a gate for the block co-oligomer to have potential applications in organic electronic devices.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yongmei Lu,Lecheng Liang,Shao Ye,Zheng Chen,Weiyue Zhao,Zhiming Cui
The sluggish kinetics of methanol oxidation reaction (MOR) and poor long-term durability of catalysts are the main restrictions of the large-scale applications of direct methanol fuel cells (DMFCs). Herein, we demonstrated an inspirational ternary Pt3Sn0.5Mn0.5/DMC intermetallic catalyst that reached 4.78 mA cm–2 and 2.39 A mg–1Pt for methanol oxidation, which were 2.50/2.44 and 5.62/5.31 times that of commercial PtRu/C and Pt/C. After the durability test, Pt3Sn0.5Mn0.5/DMC presented a very low current density attenuation (38.5%), which was significantly lower than those for commercial PtRu/C catalyst (84.2%) and Pt/C (93.1%). Density functional theory (DFT) calculations revealed that the coregulation of Sn and Mn altered the surface electronic structure and endowed Pt3Sn0.5Mn0.5 with selective adsorption of Pt for CO and Sn for OH, which optimized the adsorption strength for intermediates and improved the reaction kinetics of MOR. Beyond offering an advanced electrocatalyst, this study provided a new point of view for the rational design of superior methanol oxidation catalysts for DMFC.
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Journal of Energy Chemistry
·
2024
·
IF 14
Shilin Fan,Bin Zhu,Xiao Yu,Yang Gao,Weiping Xie,Yong Yang,Jian Zhang,Chunlin Chen
Biomass, derived from plant photosynthesis that captures carbon dioxide to form carbohydrates, offers vast renewable reserves. The electrooxidation of biomass, coupled with the hydrogen evolution reaction, enables the simultaneous production of biomass-based plastic monomers and green hydrogen, attracting significant scholarly interest. However, ambiguity remains regarding the adsorption mechanism at the catalyst surface (Langmuir-Hinshelwood or Eley-Rideal) and the adsorbed substrate groups. To address this, we prepared a Ni/Co electrode for the electrooxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) through a corrosion reaction and electro-reduction pathway. HMF conversion reached 100.00%, FDCA yield reached 96.82%, and Faradic efficiency (FE) reached 92.14%. Meaningfully, utilizing in-situ spectroscopy and electrochemical methods, this work provided valuable insights into active sites and catalyst surface adsorption.
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LANGMUIR
·
2025
·
IF 3.9
Junsheng Wang,Gege He,Jinke Shen,Xiaozhen Lv,Hongyu Mi,Shun Lu
Transition metal and nitrogen codoped graphitic carbon materials with Co–N bonds serve as key non-noble-metal catalysts for the oxygen evolution reaction (OER). To enhance catalytic efficiency, we explore the anchoring of Co–N bonds on nitrogen-doped graphitic carbon (NC) substrates with varied phosphorus content. The catalyst is synthesized through a straightforward sintering and phosphating process of ZIF@DCA in a tube furnace. X-ray photoelectron spectroscopy (XPS) demonstrated that the Co–N bonds effectively formed an efficient charge transfer channel, removing the barrier that separated the Co–N active site from the work electrode surface. Phosphorus is uniformly distributed across the Co–N substrate, ensuring the exposure of most Co–N active sites during the electrochemical reaction. With favorable structural and electronic attributes, P/Co–N-2 showcases the lowest overpotentials at 10 and 300 mA cm–2, which are 200 and 300 mV, respectively. Additionally, it demonstrates stable performance over 100 h in 1 M KOH, outperforming other similar materials and RuO2. This study offers critical insights for the rational design of Co–N structures, exploring the interplay between structure, composition, and activity in electrochemical reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yize Zhao,Xing Li,Chengkun Zhao,Yujiang Fan,Ganjun Feng,Yong Sun
Endogenous regeneration of the nucleus pulposus (NP) is hindered by inefficient recruitment of stem/progenitor cells, limited control over differentiation, and poor matrix maintenance. Here, we developed a microsphere-based platform (GBKE) that transforms upon mild hydration into a dynamic, self-healing hydrogel, allowing in situ gelation and stable retention within soft tissues. The hydrogel forms a highly porous, interconnected network that facilitates nutrient transport and deep cellular infiltration. The microspheres form an interpenetrating network structure by co-assembling through β-sheet/π-π stacking driven self-assembly, combining gelatin methacrylamide (GelMA) with the self-assembling small molecule BPAA-GFF. The chondrogenic-inducing small molecule kartogenin is bound to the BPAA-GFF nanofiber network through non-covalent interactions such as hydrogen bonds and hydrophobic forces, achieving sustained inducing effect. The MSC affinity peptide E7 is covalently coupled to the surface of the microspheres to achieve targeted cell homing. Thanks to the enhanced effect of the nanofiber network induced by BPAA-GFF, the storage modulus (≈1700 Pa) and critical shear stress (≈35 Pa) of the microgels are significantly higher than those of pure GelMA microgel. In vivo, GBKE microgels significantly improved disc height index and extracellular matrix restoration in rat models, maintaining NP regeneration for at least 8 weeks. In rabbit models, MRI analyses and histological results confirmed durable structural and functional repair for up to 12 weeks. This system enables the programmed regulation of endogenous cell behavior, offering a promising approach for minimally invasive intervertebral disc repair.
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JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Qi Lun,Tu Dan,Shi Yu,Liu Jingjing,Zhao Xinyuan,Xu Jianhua,Yang Yajie,Yang Wenyao
Zeolitic imidazolate frameworks (ZIFs) have greatly attracted attention in supercapacitors research due to their porosity and structural controllability. In this paper, a series of Co–nitrogen carbon (Co–NCs) were obtained via a facile one-step calcination process using 3D star-shaped Co–ZIF as a precursor. The energy storage mechanism is analyzed and it is concluded that Co–NCs show excellent capacitance and cycling stability, attributed to its star-shaped porous morphology and high pseudocapacitance contribution. The optimized Co–NCs/550 exhibits a specific capacity of 825 F g −1 at a current density of 0.1 A g −1 , and a highly stable cycling performance over 5000 cycles at a current density of 2 A g −1 . This work provides a practical strategy for designing stable electrode for high-performance supercapacitors.
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Chem
·
2024
·
IF 19.1
Xiaoran Zhang,Xiaorong Zhu,Shuowen Bo,Chen Chen,Qingfeng Zhai,Shuang Li,Xiaojin Tu,Jianyun Zheng,Dongdong Wang,Xiaoxiao Wei,Wei Chen,Tehua Wang,Yafei Li,Qinghua Liu,San Ping Jiang,Liming Dai,Shuangyin Wang
Electrocatalysis offers a sustainable approach to artificial nitrogen fixation yet faces numerous challenges. Selective synthesis of nitrogen-containing compounds shows promise but needs significant improvement. Herein, we demonstrate selective ammonia and urea synthesis via co-electrolysis with CO 2 . High CO binding energy on Re-Mn catalysts leads to the formation of ∗C species, which serve as electron reservoirs to enhance N 2 activation for C-N coupling (N 2 + ∗C → ∗CN 2 ), followed by C-N dissociation. This results in ammonia production with a yield rate of 48.9 ± 2.4 mg g −1 h −1 and an N-selectivity of 98.4%. In contrast, Zn-Mn sites, characterized by low CO binding, facilitate the migration of CO and its coupling with adsorbed N 2 (CO + ∗N=N∗ → ∗NCON∗). Subsequent hydrogenations of ∗NCON∗ promote urea synthesis with an N-selectivity of 89.1%. Utilizing Janus coupling with two C-N pathways aims to meet energy, agriculture, and chemical industry demands. We realized the selective synthesis of ammonia and urea, respectively, in one electrocatalytic system for the first time by Janus coupling with two distinguishable C-N coupling paths from N 2 and CO 2 .
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ADVANCED MATERIALS
·
2020
·Vol. 32
·期 39
·2002382
·
IF 27.398
Changming Zhao,Gan Luo,Xiaokang Liu,Wei Zhang,Zhijun Li,Qian Xu,Qinghua Zhang,Huijuan Wang,Deming Li,Fangyao Zhou,Yunteng Qu,Xiao Han,Zezhou Zhu,Geng Wu,Jing Wang,Junfa Zhu,Tao Yao,Yafei Li,Henny J.M. Bouwmeester,Yuen Wu
Electrochemical reduction of CO to value-added products holds promise for storage of energy from renewable sources. Copper can convert CO into multi-carbon (C 2+ ) products during CO electroreduction. However, developing a Cu electrocatalyst with a high selectivity for CO reduction and desirable production rates for C 2+ products remains challenging. Herein, highly lattice-disordered Cu 3 N with abundant twin structures as a precursor electrocatalyst is examined for CO reduction. Through in situ activation during the CO reduction reaction (CORR) and concomitant release of nitrogen, the obtained metallic Cu° catalyst particles inherit the lattice dislocations present in the parent Cu 3 N lattice. The de-nitrified catalyst delivers an unprecedented C 2+ Faradaic efficiency of over 90% at a current density of 727 mA cm −2 in a flow cell system. Using a membrane electrode assembly (MEA) electrolyzer with a solid-state electrolyte (SSE), a 17.4 vol% ethylene stream and liquid streams with concentration of 1.45 m and 230 × 10 −3 m C 2+ products at the outlet of the cathode and SSE-containment layer are obtained.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Liang Fu,Zhenping Qu,Lingling Zhou,Yue Ding
Interface engineering is demonstrated to lead to significant improvement in the catalytic performance for electrochemical CO 2 reduction reactions (CO 2 RR). In this work, we demonstrate a heterogeneous In(OH) 3 -Ag interface catalyst in which the appropriate In(OH) 3 clusters modified on metal Ag nanoparticles surface greatly improves the CO selectivity in CO 2 RR, realizing a CO faradaic efficiency (FE CO ) of 93% at − 0.7 V vs. RHE. The performance enhancement is attributed to the preferentially CO 2 adsorption and activation by the In(OH) 3 -Ag interface sites. In situ Raman spectroscopy reveals that the formation of In(OH) 3 -Ag interface sites is significantly favorable for the generation of key *CO 2 − intermediate at low overpotential. Further theoretical calculation confirms that the In(OH) 3 -Ag interface could enhance the adsorption of *COOH species on catalyst by means of tailoring the surface properties and electronic structures. This work shows that hydroxide-metal interface engineering is a promising pathway to regulate the activity for selective CO 2 RR properties.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Xiangzhi Wang,Jing Wang,Zelong Li,Muhan Yang,Arbaz Rehman
Pharmaceuticals and personal care products (PPCPs), known for their severe ecological risks, are frequently detected in coastal waters worldwide. However, the environmental fate in marine systems remains poorly understood. This study investigated the co-metabolic degradation mechanism of a typical PPCP, sulfamethoxazole (SMX), by a marine consortium SAB using alginate—a natural organic matter—as a co-substrate, aiming to elucidate the biodegradation process of PPCPs in actual marine environments. An integrated approach, including metagenomic sequencing (with binning), RT-qPCR, molecular docking, metabolic modeling, and metabolomics, was employed. Results demonstrated that the SAB consortium efficiently degraded SMX at concentrations from 50 μg/L to 10 mg/L, achieving over 96% removal within 24 h. SMX degradation was achieved through metabolic cross-feeding of alginate by key species within the SAB consortium. Specifically, alginate is initially converted by Vibrio into the central metabolite 2-keto-3-deoxy-D-gluconate (KDG). KDG is subsequently metabolized by Tritonibacter , Halopseudomonas , and Vibrio , generating key metabolites such as acetyl-CoA, serine, cysteine, and guanine. These metabolites support microbial growth and induce production of SMX-degrading enzymes, such as threonine dehydratase, cysteine S-conjugate β-lyase, and guanine deaminase, leading to SMX cleavage and mineralization. Additionally, acetyl-CoA provides acetyl groups for arylamine N-acetyltransferase-mediated SMX acetylation. These processes collectively drive the co-metabolic degradation of SMX. Overall, this study provides critical insights into PPCPs' fate in marine environments.
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RSC Advances
·
2018
·Vol. 8
·期 34
·18966-18971
·
IF 2.936
Zhiwei Lu,Yujuan Chen,Zhaoen Liu,Aoqi Li,Dong Sun,Kelei Zhuo
The development of high energy density and power density supercapacitors is very necessary in energy storage and application fields. A key factor of such devices is high-performance electrode materials. In this work, nitrogen and sulfur co-doped graphene aerogels (N/S-GA) were synthesized using graphene oxide as the precursor and 2-mercapto-1-methylimidazole as both the reducing agent and the N/S doping agent. The pore size distribution of the as-prepared N/S-GA was measured and the N/S-GA possesses a hierarchical porous structure. As an electrode material of supercapacitors, the N/S-GA could provide a suitable structure for charge accommodation and a short distance for ion transport. When 1-ethyl-3-methylimidazolium tetrafluoroborate ([Emim]BF4) ionic liquid was used as the electrolyte, the specific capacitance of the N/S-GA electrode material reached 212 F g−1 and 162 F g−1 at the current densities of 1 A g−1 and 10 A g−1, respectively. And the energy density and average power density of the N/S-GA based supercapacitor could reach 117 W h kg−1 and 1.0 kW kg−1 at 1 A g−1, 82 W h kg−1 and 9.5 kW kg−1 at 10 A g−1, respectively. It is believed that the N/S-GA material can be used in high-performance supercapacitors.
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POLYMER SCIENCE SERIES B
·
2025
·Vol. 67
·期 2
·15
·
IF 1
Zhijun Li,Huang Zhengyong,Xing Ruiguang
In this study, the preparation of diphenylsilylene diol (DP)-modified double-A epoxy resin (E51) with resveratrol-functionalized graphene (Res/rGO) composites and their performance characterization were investigated. Firstly, the double-A epoxy resin (EP) was modified with DP to improve its mechanical properties and thermal stability. Then, Res/rGO was introduced into the modified epoxy resin (DP/E51), and a series of modified epoxy resin/resveratrol functionalized graphene (Res/rGO-DP/E51) composites were prepared. The effects of different graphene contents on the mechanical properties of the materials were analyzed by conducting tensile property tests on the composites. The results showed that the DP-modified epoxy resin exhibited a significant improvement in tensile strength, especially after the introduction of an appropriate amount of Res/rGO, the tensile properties of the composites were further optimized. Resveratrol, as a natural antioxidant substance, significantly improved the interfacial bonding and dispersion of the composites after functionalization on the graphene surface, thus enhancing the overall performance of the composites. In addition, the Res/rGO-DP/E51 composites exhibited excellent thermal stability, which has a good application prospect.
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