NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 12
·5456-5464
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IF 2.7
Yanhua Gao,Dongfeng Zhang,Hongya Liu,Ying Chen,Yuning Liang,Mingchun Bi,Juan Ren,Zhihua Wang
Based on the anion exchange strategy, a novel Bi2S3/BiOCl0.1Br0.9 S-scheme heterojunction was prepared via a facile one-step low-temperature water bath method for the first time. In this process, 2D Bi2S3 nanosheets were controllably grown on the surface of a 3D hollow BiOCl0.1Br0.9 solid solution. Under visible light irradiation, the as-prepared 3BS-BCB exhibited a remarkable photocatalytic degradation efficiency of 99.67% toward rhodamine B (Rh B) within 140 min, which is approximately 3.57 times higher than that of the BiOCl0.1Br0.9 solid solution alone. The enhanced photocatalytic performance is attributed to the formation of an interfacial electric field (IEF), which accelerated the separation rate of photoinduced electron–hole pairs and coupled the strong redox ability of both the semiconductors. Moreover, the photosensitive effect of Bi2S3 extended its light absorption range, increasing the yield of photogenerated charge carriers. Such thermodynamic and kinetic compatibility is the fundamental reason for the enhanced photocatalytic efficiency. This study provides new insights into the design of S-scheme heterojunction photocatalysts with visible light response and high redox ability based on wide-band gap semiconductors.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Xiaofei Lei,Wenjuan Li,Kanjun Sun,Sitong Liu,Aoji Liang,Hui Peng,Guofu Ma
Transition metal sulfides embedded in co-doped porous carbon materials with nitrogen and sulfur are a promising catalyst that can effectively solve the problem of slow oxygen reduction reaction (ORR) kinetics. However, monometallic sulfides consisting of a single active component only have monofunctional catalytic activity and cannot effectively increase the rate of oxygen evolution reaction (OER), thus limiting the energy conversion efficiency of Zn-air batteries (ZAB). Herein, a unique silica template assisted in situ pyrolysis strategy is used to synthesize iron (Fe)-doped cobalt sulfide (Co 9 S 8 ) nanoparticle embedded in a honeycomb nitrogen (N), sulphur (S) co-doped porous carbon (Fe/Co 9 S 8 @NSC) electrocatalyst. The introduction of Fe increases the active component of the catalyst and further enhances the catalytic ability of Co 9 S 8 by optimizing the electronic structure through charge transfer effect. Therefore, the rich active sites of Fe/Co 9 S 8 nanoparticles anchored in N, S co-doped carbon materials with rich pore structure enable the catalysts to have good bifunctional catalytic activities of ORR and OER. In particular, the Fe/Co 9 S 8 @NSC has a high half-wave potential of 0.82 V for catalytic ORR and only needs low overpotential of 332 mV at a current density of 10 mA cm −2 for catalytic OER. In addition, the Fe/Co 9 S 8 @NSC catalyst based rechargeable ZAB also exhibits a significant specific capacity of 734 mAh g −1 and prolonged stability of 270 h, which outperforms the bulk of recently reported catalysts based on transition metal sulfides-based catalysts. This research offers a workable method for producing metal sulfides catalysts with bifunctional catalytic activity.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Linsen Li,Zhuwei Yang,Hui Xiong,Ming Ma,Riguang Zhang,Zhao Jiang
The NECZ/12H-NECZ (N-ethylcarbazole/dodecahydro-N-ethylcarbazole) system is one of the commercially promising liquid organic hydrogen carriers (LOHCs). However, the dehydrogenation reaction of 12H-NECZ is still the bottleneck of the whole hydrogen storage and release process, possessing a relatively low hydrogen release rate. In this study, one kind of C3N4 (carbon nitride) mesoporous nanosheet material with abundant N vacancies was fabricated by the thermal treatment of trace S-doped C3N4, and a series of Pd-based catalysts were prepared by the impregnation reduction method. The Pd/S0.03-C3N4-Nv550 (treated by S-doped and N) catalyst with abundant N vacancies showcases the most outstanding catalytic performance, achieving a 5.41 wt % hydrogen release amount as well as 81.09% NECZ selectivity at 90 min. Combined with the experimental and computational results, the presence of trace S does not lead to structural collapse of the material and interestingly induces the generation of high concentrations of N vacancies. The N vacancies greatly facilitate the dispersion of loaded metals, offering more active sites; meanwhile, the existence of N vacancy weakens the electronic localization of C3N4 carriers, modulates the electronic structure of active metal Pd, and promotes the activation of reactants and intermediates. What is more, the Pd/S0.03-C3N4-Nv550 catalyst shows excellent stability during long-term cycle tests. It provides some reference values for the design of LOHC dehydrogenation catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Manman Mu,Lingqi Meng,Siting Ma,Wenjuan Chen,Xiaohong Yin,Guoyi Bai
Covalent organic frameworks (COFs) equipped with controllable porosity and excellent structural stability are regarded as promising candidates for photocatalytic CO 2 reduction, yet some inherent drawbacks including low CO 2 activation and sluggish charge carriers’ transfer properties urgently need to be addressed. Herein, we developed an imine-bridged strategy to construct ZnO/COF heterostructure by integrating donor–acceptor COF (TAPT-DMTP COF) on the surface of amino-modified ZnO for photocatalytic CO 2 reduction. The optimal photocatalyst, N ZnO/TAPT-DMTP COF-3, exhibited superior photocatalytic activity for reducing CO 2 to CO and CH 4 , which was significantly higher than pristine COF and non-covalently bridged ZnO/TAPT-DMTP COF. Experimental and photo-electrochemical results reveal that the microstructure of TAPT-DMTP COF, interfacial imine-bridging and S-scheme heterojunction play a crucial role in promoting photoinduced charge transfer and separation, thus improving photocatalytic efficiency. Moreover, in-situ characterization and theoretical calculations indicate the photoinduced electrons transfer from N ZnO to TAPT-DMTP COF upon hybridization, and this S-scheme heterostructure dramatically lowers the energy barrier of rate-determining step from *COOH to *CO. This work provides insight into the covalent-linked COF-based S-scheme photocatalyst and highlights its vital role in enhancing CO 2 reduction.
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FUEL
·
2025
·
IF 7.5
Ruotong Cui,Wenlong Xu,Yanpeng Zhang,Jingxian Wang,Yingyun Qiao,Yuanyu Tian
Identifying and analyzing the reaction process of S atoms in coal at the molecular level has been a key and difficult problem in coal chemistry. Here, we used dibenzyl sulfide as a model compound for S-containing substances in coal and predicted the pyrolysis process of C-S in coal through the pyrolysis products, which indicated that the C-S bond would be broken firstly above the energetic basis point to generate intermediate S-containing radicals. A hydrogen-donating solvent (9, 10-dihydroanthracene) was utilized as the radical trapping agent to reveal the S-containing radical reaction process through the changes of the products before and after the trapping reaction. Density functional theory was further used to calculate the pyrolysis process to help verify the radical history of the response. Finally, pyrolysis experiments were performed on raw coal to confirm the generality of the pyrolytic radical regulatory mechanism of C-S. This study identifies and analyzes the relationship between C-S structure and reactivity during coal pyrolysis at the molecular level, and confirms the universal law of raw coal’s pyrolytic radical reaction mechanism. This not only provides theoretical guidance and a basis for the free radical regulation process during the pyrolysis of S-containing structures in coal but also provides theoretical support for the clean and efficient utilization of coal.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yansheng Liu,Yongquan Wei,Guofu Wang,Xiaobo Jia,Jin Zhou,Hongqi Li,Haixin Chang,Zhaoxu Li
Surface-enhanced Raman scattering (SERS) spectroscopy plays an important role in enabling high-precision detection and non-invasive diagnostics. Periodic metallic nanostructures with strong electromagnetic fields and tunable localized surface plasmon resonance can achieve high SERS sensitivity, but fabricating such nanostructures remains a challenge. In this work, the anodic aluminum oxide (AAO) nanocavity template-assisted process of fabricating periodic nanostructures with modulating morphologies from Ag nanoclaws (AgNCWs) to Ag nanocones (AgNCEs) is proposed. The morphologies-related SERS performances of nanostructures are analyzed by using rhodamine 6 g (R6G) as a probe molecule and the optimized AgNCEs possess a limit of detection (LOD) of 1 × 10 −9 M. A sandwich strategy is applied to detect SARS-CoV-2 S protein in phosphate-buffered saline (PBS) and pharyngeal swab solution (PSS). The ACE2-modified AgNCEs (ACE2/AgNCEs) structure is applied to bind to the SARS-CoV-2 S protein. The 4-MBA and SARS-CoV-2 S antibody functionalized Au nanoparticles (AuNPs) are used as nanotags. By forming the ACE2/AgNCEs-SARS-CoV-2 S protein-nanotags sandwich structure, characteristic peak intensities of 1580 cm −1 are used as the report signal, and the LOD for SARS-CoV-2 S protein in PBS and PSS solution are 10 fg/mL.
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Small
·
2024
·Vol. 20
·期 29
·2310087
·
IF 13
Yunfeng Qiu,Yongxia Zhang,Miao Yu,Xinyi Li,Yanxia Wang,Zhuo Ma,Shaoqin Liu
Simultaneously improving electrochemical activity and stability is a long-term goal for water splitting. Herein, hierarchical N-doped carbon nanotubes on carbon nanowires derived from PPy are grown on carbon cloth, serving as a support for NiCo oxides/sulfides. The hierarchical electrodes annealed in N 2 or H 2 /N 2 display improved intrinsic activity and stability for hydrogen evolution reaction (HER) and glucose oxidation reaction. Compared with Pt/C||Ir/C in alkaline media, the glucose electrolysis assembled with electrodes exhibits a cell voltage of 1.38 V at 10 mA cm −2 , durability for >12 h at 50 mA cm −2 , and resistance to glucose/gluconic acid poisoning. In addition, electrocatalysts can also be applied in ethanol oxidation reactions. Systematic characterizations reveal the strong interactions between NiCo and N-doped carbon support-induced partial charge transfer at the interface and regulate the local electronic structure of active sites. Density functional theory calculations demonstrate that the synergistic effect between N-doped carbon supports, metallic NiCo, and NiCo oxides/sulfides optimize the adsorption energy of H 2 O and the H* free energy for HER. The energy barrier of the dehydrogenation of glucose effectively decreased. This work will attract attention to the role of metal-support interactions in enhancing the intrinsic activity and stability of electrocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ming Li,Xuemeng Zhang,Dongqing Wang,Xiaofei Fan,Qianyong Cao,Huining Xiao,Shiwei Guo,Chungang Yuan,Yuling Zhang
Nanofiltration membranes are extensively implemented in water treatment, particularly for the efficient interception of toxic heavy metal ions. This work introduces a novel functional membrane fabricated via interfacial polymerization, incorporating nitrogen and sulfur co-doped carbon dots (N, S-CDs) as additives to enhance mercury removal from aqueous solutions. The integration of carbon dots has been demonstrated to significantly augment the membrane’s hydrophilicity, thereby improving the pure water flux. Moreover, it modulates the crosslinking degree of the polyamide layer, enhancing mercury retention. The N, S-CDs, due to their high selectivity for Hg (II), confer the modified membrane with fluorescence detection capabilities, allowing for the precise quantification of mercury rejection. The membrane achieved a remarkable Hg (II) retention rate of 94.85 %, with a pure water flux of 10.68 L m −2 h −1 bar −1 , and attained a detection limit of 5.49 × 10 −7 M for Hg (II). The durability and reusability of the membrane are substantiated by soaking and recycling trials, underscoring the stable encapsulation of N, S-CDs within the nanofiltration matrix.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Jun He,Haoran Qian,Guodong Peng,Hongyu Hu,Li Jiang,Xiaojun He
It is a big challenge to tune the structure and composition of carbon-based anode materials to increase the active sites by a green synthesis strategy for potassium ion batteries (PIBs). Herein, the N/F/S co-doped three-dimensional (3D) interconnected carbon nanosheets (NFS-CNSs) were synthesized from coal tar pitch (CTP) through a green and low-temperature treatment process for the first time. The as-obtained NFS-CNS 600 features 3D interconnected ultra-thin carbon nanosheets with abundant active sites, tunable N/F/S species, and enlarged carbon interlayer spacing. The density functional theory calculation results demonstrate that NFS-CNSs exhibit the highest electron density and most negative K + adsorption energy (–0.59 eV) compared to single or double-atom doping, thereby enhancing the storage performance of K + . As an anode for PIBs, the NFS-CNS 600 exhibits good cycle stability (98.2 % capacity retention after 200 cycles at 0.2 A g −1 ), high capacity (409.1 mAh g −1 at 0.05 A g −1 ) and rate performance (179.5 mAh g −1 at 5 A g −1 ). Besides, the NFS-CNS 600 anode also displays outstanding sodium storage performance. This work offers a green strategy to synthesize CTP-based anode materials from coal chemical by-products for high-performance PIBs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Guizhen Liu,Shanshan Zhang,Yutian Cai,Yongzhi Cheng,Yingli Zhu,Pingan Chen,Hui Luo,Xiangcheng Li,Fu Chen
Flexible manipulations of morphology and composition have been considered as an art to achieve excellent microwave absorption performance for absorbers derived from metal-organic frameworks (MOFs). In this work, a strategy combining ligand-exchange induced hollow engineering and high-temperature one-step sulfuration has been proposed to fabricate the Co 9 S 8 /Co@N, S dual-doped carbon-based absorbers with tailored solid, yolk-shelled and entirely hollow polyhedral morphologies. The progressive hollow engineering not only enables composition control in the sulfuration process, but also endows the proposed absorbers with superior microwave absorption capacity due to the enhanced conductivity loss and Maxwell-Wagner polarization as well as optimized impedance matching. The yolk-shelled Co 9 S 8 /Co@N, S dual-doped carbon-based composite achieves a broad effective absorption bandwidth of 5.13 GHz at 1.88 mm with 20 wt% loading and realizes a minimum microwave loss of − 51.78 dB @ 11.63 GHz with 2.37 mm. This work reveals that the joint strategy of ligand-exchange induced hollow engineering and gas-solid reactive thermal process is an effective path to construct high-efficient lightweight multi-interfacial microwave absorbers for addressing the electromagnetic pollutions.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Xiaoyan Lu,Xinhui Jiang,Jindou Hu,Junhong Li,Anjie Liu,Zhenjiang Lu,Jing Xie,Yali Cao
The p–n type charge transfer pathway plays an active role in efficient carrier separation and enhancement of photocatalytic activity, but it will also reduce the redox ability of photogenerated carriers. Herein, the anchored amino molecular layer acts as a heterojunction conversion switch to transform Cu2O/T-N from a p–n to an S-scheme heterojunction. Following this transformation, the redox ability of carriers can be dramatically enhanced: the reduction potential of photogenerated electrons increases from −0.49 eV to −1.68 eV, and the oxidation potential of photogenerated holes increases from 0.32 eV to 2.33 eV. Therefore, the optimized Cu2O/T-N S-scheme heterojunction photocatalyst exhibits superior photocatalytic performance for hydrogen evolution (up to 41.85 mmol g−1, 64 times higher than that of pure TiO2) and nitrogen fixation (as high as 18 mmol gCu2O−1 h−1). Moreover, the post-conversion carrier transfer pathway also prevents the accumulation of holes on Cu2O, alleviating the photocorrosion caused by hole oxidation. Hence, the catalytic activity remains stable during photocatalytic cycling for up to 50 h. This study provides a straightforward and practical method for enhancing the redox capacity of photocatalysts.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Xia Liu,Ming Chen,Dengjun Wang,Feng Du,Nan Xu,Wu Sun,Zhaoxiang Han
Iron-based materials such as nanoscale zerovalent iron (nZVI) are effective candidates to in situ remediate hexachromium (Cr(VI))-contaminated groundwater . The anaerobic bacteria could influence the remediation efficiency of Cr(VI) during its cotransport with nZVI in porous media . To address this issue, the present study investigated the adsorption and reduction of Cr(VI) during its cotransport with green tea (GT) modified nZVI (nZVI@GT) and iron sulfides (FeS and FeS 2 ) in the presence of D. vulgaris or S. putrefaciens in water-saturated sand columns. Experimental results showed that the nZVI@GT preferred to heteroaggregate with FeS 2 rather than FeS, forming nZVI@GT-FeS 2 heteroaggregates. Although the presence of D. vulgaris further induced nZVI@GT-FeS 2 heteroaggregates to form larger clusters, it pronouncedly improved the dissolution of FeS and FeS 2 for more Cr(VI) reduction associated with lower Cr(VI) flux through sand. In contrast, S. putrefaciens could promote the dispersion of the heteroaggregates of nZVI@GT-FeS 2 and the homoaggregates of nZVI@GT or FeS by adsorption on the extracellular polymeric substances , leading to the improved transport of Fe-based materials for a much higher Cr(VI) immobilization in sand media. Overall, our study provides the essential perspectives into a chem-biological remediation technique through the synergistic removal of Cr(VI) by nZVI@GT and FeS in contaminated groundwater. Environmental implication The green-synthesized nano-zero-valent iron particles (nZVI@GT) using plant extracts (or iron sulfides) have been used for in situ remediation of Cr(VI) contaminated groundwater. Nevertheless, the removal of Cr(VI) (including Cr(VI) adsorption and Cr(III) generation) could be influenced by the anaerobic bacteria governing the transport of engineered nanoparticles in groundwater. This study aims to reveal the inherent mechanisms of D. vulgaris and S. putrefaciens governing the cotransport of nZVI@GT combined with FeS (or FeS 2 ) to further influence the Cr(VI) removal in simulated complex groundwater media. Our findings provides a chemical and biological synergistic remediation strategy for nZVI@GT application in Cr(VI)-contaminated groundwater.
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