CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Maonan Ran,Guan Zhang
The NO 3 − electroreduction process presents a promising alternative to the Haber-Bosch method by offering dual benefits: removal of nitrates from wastewater coupled with efficient NH 3 production. Herein, Mo and S doped Fe 3 O 4 nanoplates grown on foam Fe (Mo-S-Fe 3 O 4 @FF) with electron-rich Mo δ+ state was synthesized through a facile hydrothermal approach. Notably, Mo-S-Fe 3 O 4 @FF electrode achieved a nearly fourfold enhancement in ammonium yield compared to foam Fe electrode, while also enhancing the NH 3 Faradaic efficiency. At − 1.3 V vs . Ag/AgCl in a K 2 SO 4 + KNO 3 solution, the Mo-S-Fe 3 O 4 @FF electrode attained a NH 3 Faradaic efficiency of 91.3 %. Furthermore, performance was observed to improve with increasing solution pH levels as the reaction proceeded. From both kinetic and thermodynamic perspectives, our findings demonstrate that high NH 3 production activity is characteristic of Mo-S-Fe 3 O 4 @FF—indicating significant enhancements in conversion rates from NO 3 − →NO 2 − →NH 3 . Theoretical calculation, in conjunction with experimental analyses, reveal that the co-modification of Fe 3 O 4 with Mo and S enhances electron transfer capacity during NO 3 − RR. This modification forms Lewis-acid (Fe-Mo) pairs that increase nitrate adsorption energy alongside Lewis-base (S-O) sites that attract protons, thereby improving overall NO 3 − RR activity. This report elucidates the synergistic effects of Lewis-acid and Lewis-base sites on optimizing catalytic performance for NO 3 − RR using foam Fe-based electrodes.
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RENEWABLE ENERGY
·
2025
·
IF 9.1
Lina Dai,He Wang,Liru Cui,Yanduo Liu
Single photocatalysts face problems such as easy recombination of photo-generated charge carriers, weak oxidation-reduction ability, and narrow spectral response range, which greatly restrict their practical applications in energy and environmental fields. This article constructs a new type of Cu-Co Prussian blue analogues S-scheme photocatalytic material. The material is composed of oxidized photocatalysts (Ag 3 PO 4 ) and reduced photocatalysts (Cu-Co PBAs). By utilizing the characteristics of Cu-Co Prussian blue analogues photocatalysts, such as high conduction band position, rich catalytic sites, and small band gap, photocatalytic efficiency can be significantly enhanced. The CO production rate is 36.3 μmol/g/h, and the selectivity can reach 93.8 %, which is far superior to the current mainstream photocatalytic system. By studying the construction method and CO 2 reduction performance of the composite photocatalyst, the structure-performance relationship is clarified. The steady-state photocurrent spectroscopy reveals the S-scheme mechanism photocarrier transfer and separation kinetics. Techniques such as near-ambient pressure X-ray photoelectron spectroscopy reveal the interface electron transfer mechanism. In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy and Density Functional Theory calculations are used to study the formation of reaction intermediates and reveal the catalytic mechanism. This study will offer critical understanding for advancing developments of selective photocatalysts aimed at sustainable CO 2 utilization.
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Wei Jiang,Zhaomei Wu,Yingming Zhu,Wen Tian,Bin Liang
Four silver chalcogen compounds, Ag 2 O, Ag 2 S, Ag 2 Se and Ag 2 Te, can be utilized as visible-light-driven photocatalysts. In this research, the electronic structures of these compounds were analyzed by simulation and experiments to systematically reveal the relationship between photocatalytic performance and energetic structure. All four chalcogenides exhibited interesting photocatalytic activities under ultraviolet, visible and near-infrared light. However, their photocatalytic performances and stability significantly depended on the band gap width, and the valence band and conduct band position, which was determined by their composition. Increasing the X atomic number from O to Te resulted in the upward movement of the valence band top and the conduct band bottom, which resulted in narrower band gaps, a wider absorption spectrum, a weaker photo-oxidization capacity, a higher recombination probability of hole and electron pairs, lower quantum efficiency, and worse stability. Among them, Ag 2 O has the highest photocatalytic performance and stability due to its widest band gap and lowest position of VB and CB. The combined action of photogenerated holes and different radicals, depending on the different electronic structures, including anion ozone radical, hydroxide radical, and superoxide radical, was observed and understood. The results of experimental observations and simulations of the four silver chalcogen compounds suggested that a proper electronic structure is necessary to obtain a balance between photocatalytic performance and absorbable light region in the development of new photocatalysts.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 39
·22463-22474
·
IF 10.733
Qian Lu,Xiaohong Zou,Ran Ran,Wei Zhou,Kaiming Liao,Zongping Shao
Lithium–sulfur (Li–S) batteries are of great interest due to their high theoretical energy density and potentially low cost. However, two of the key issues hindering their commercialization are the polysulfide shuttling and Li-dendrite growth, which result in severe capacity decay and serious safety hazards. Herein, liquid-phase delaminated birnessite (HxMnO2+x) nanosheets along with graphene and carbon nanotubes are utilized for the first time to create an “electronegative” coating layer for Li–S batteries to suppress the polysulfide shuttling and Li-dendrite growth. The as-prepared coating layer enables stable cycling of the Li–S battery with a low capacity decay rate of 0.04% per cycle over 1000 cycles at 1C. In addition, a Li-symmetrical cell with the coating layer shows suppressed dendrite growth even after being cycled over 1000 hours at 1 mA cm−2. This excellent performance is ascribed, in part, to the synergistic effect of the chemical and electrostatic interactions among polysulfides, Li ions, and [MnO2+x]x− ions, resulting in a homogeneous Li-ion flux distribution and a mitigated polysulfide shuttling. The proposed concept of an “electronegative” bifunctional coating layer illustrates a simple and effective way to develop highly stable and safe Li–S batteries.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Yu Lin,Fangfang Li,Xiaoqing Li,Hongwei Zhao,Gang Liu
To recycle wastes and develop renewable energy, much effort has been focused on converting biowastes into porous carbon for supercapacitors. Porous nanocage-like carbons have excellent capacitive properties, but generally their preparation methods are costly or complex. Herein, a “one-step” strategy of synchronous activation and support through the thermal decomposition of a multifunctional template (magnesium acetate, Mg(Ac)2) is designed to prepare N-, O-, and S-codoped mesoporous hollow biochar nanocages (BNC-700). The BNC-700 prepared displays an interconnected porous structure and a two-dimensional (2D) multilayer wall/three-dimensional (3D) hollow nanocage structure with abundant active heteroatoms and edge defects. Due to their specific structures, high surface areas (1369 m2 g–1), and large pore volumes (1.81 cm3 g–1), the assembled supercapacitor delivers a considerable energy density of 37.4 Wh kg–1 at 212 W kg–1 and cycling stability of 99.5% after 15,000 cycles. The unique structure and N, O, and S codoping characteristics ensure a potential application for BNC-700 in supercapacitors. In summary, a strategy is designed for the green, simple, and cost-effective preparation of high-performance biochar for advanced energy storage devices.
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高影响因子
ANALYTICAL CHEMISTRY
·
2018
·
IF 6.042
Dongxia Chen,Jingjin Zhao,Liangliang Zhang,Rongjun Liu,Yong Huang,Chuanqing Lan,Shulin Zhao
Calcium ion (Ca2+) plays crucial roles in the signal transduction pathways associated with various physiological and pathological events. Monitoring intracellular Ca2+ is of great significance for cell biology research. Here, we report the use of biomass quantum dots (BQDs) as a fluorescent reporter for imaging of intracellular Ca2+, based on the inner-filter-mediated luminescence which was assisted by a Ca2+ chelator alizarin red S (ARS). BQDs were prepared by hydrothermal heating of capsicum. The absorption of ARS overlaps with the excitation of the BQDs, the fluorescence of BQDs being quenched through the inner-filter effect. But the absorption of Ca-ARS complex red shifts and shows a poor inner-filter effect. Thus, Ca2+ can be detected by the inner-filter-mediated luminescence using the BQDs-ARS nanohybrid system. Using the proposed nanosystem, the imaging of intracellular Ca2+ and real-time monitoring of the Ca2+ level change under histamine stimulation were also achieved. Thus, this nanosystem holds potential applications in other Ca2+-related signal transduction study.
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PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 135
·期 11
·45984
·
IF 1.86
Ying Yue,Zhihui Fan,Chang Zheng,Lan Ding,Huiying Wang,Miao Zhang,Kuilin Deng
In this investigation, a group of poly( l -malic acid acetate- co - l -lysine ester)s (PMALs) with excellent thermo-sensitivity and non-cytotoxicity were prepared by an optimized synthetic route from natural l -malic acid and l -lysine. The structure and properties of PMALs including monomers were systematically characterized by FTIR, 1 H NMR, UV, gel permeation chromatograph, scanning electron microscope, contact angle measurement, cell counting kit assess (CCK-8), and confocal laser scanning microscopy (CLSM). Three PMALs show a reversible lower critical solution temperature of 8–36 °C depending on their chemical structure. The contact angle measurement revealed a considerable discrepancy in the hydrophilicity/hydrophobicity of PMALs and further influence on their thermo-sensitivity. The viability of HeLa cells exposed to 0.2–100 μg/mL PMALs solution was found to be in a range 80–103% after 24, 48, and 72 h of incubation, indicating no cytotoxicity. Moreover, a spherical nanocarrier with core-shell structure was facilely fabricated via the thermo-sensitivity of PMALs and hydrophobicity of drug. CLSM observations manifested that the hydrophobic-curcumin-enwrapped nanocarriers can clearly internalize into the cellular inside. The sustained release of curcumin from nanocarriers in vitro provided a possibility of depressing fast hydrolytic degradation at physiological pH or other side-effects. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 45984.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Jiaxin Li,Chongchao Yao,Bo Song,Zhihao Zhang,Andreas Libonati Brock,Stefan Trapp,Jing Zhang
Microbial fuel cells (MFCs) have great promise for power generation by oxidizing organic wastewater, yet the challenge to realize high efficiency in simultaneous energy production and resource recovery remains. In this study, we designed a novel MFC anode by synthesizing S-doped NiFe 2 O 4 nanosheet arrays on carbon cloth (S10-NiFe 2 O 4 @CC) to build a three-dimensional (3D) hierarchically porous structure, with the aim to regulate the microbial community of sulfur-cycling microbes in order to enhance power production and elemental sulfur (S 0 ) recovery. The S10-NiFe 2 O 4 @CC anode obtained a faster start-up time of 2 d and the highest power density of 4.5 W/m 2 in acetate-fed and mixed bacteria-based MFCs. More importantly, sulfide removal efficiency (98.3 %) (initial concentration of 50 mg/L S 2− ) could be achieved within 3 d and sulfur (S 8 ) could be produced. Microbial community analysis revealed that the S10-NiFe 2 O 4 @CC anode markedly enriched sulfur-oxidizing bacteria (SOB) and promoted enrichment of SOB and sulfate-reducing bacteria (SRB) in the bulk solution as well, leading to the enhancement of power generation and S 0 recovery. This study shows how carefully designing and optimizing the composition and structure of the anode can lead to the enrichment of a multifunctional microbiota with excellent potential for sulfide removal and resource recovery.
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PubMed
高影响因子
MINERALS ENGINEERING
·
2025
·
IF 5
Hulin Gao,Jian Liu,Jiamei Hao,Meiguang Jiang,Xu Bai,Da Li,Rong Huang
The reduction of sulfur impurities in copper concentrates typically necessitates a highly alkaline environment generated by excessive lime addition, owing to the analogous surface flotation properties of chalcopyrite and pyrite. In this study, an innovative approach was proposed by pre-combining green reagent xanthan gum (XG) with calcium (II) ions to enhance its efficacy as a selective depressant for pyrite. Micro-flotation tests on mixed minerals revealed that XG alone exhibits no depressive effect, whereas the application of the XG-Ca at pH 9 enhances the Cu grade of the concentrate to 29.70% (from 16.43% in the raw mineral), with the recovery of chalcopyrite and pyrite being 85.31% and 12.60%, respectively. The complexation-enhanced depression mechanism of Ca on XG and the interaction mechanism between XG-Ca and pyrite surfaces were evaluated using techniques such as XPS, FTIR, TOF-SIMS, SEM-EDS, and molecular dynamics simulations. The results indicated that calcium ions primarily coordinate with carboxyl groups, inducing the extension of XG side chains and greater exposure of functional moieties, which facilitates the formation of a uniform and compact adsorption layer on pyrite surfaces. There are primarily two interaction mechanisms between XG-Ca and Pyrite: (1) The coordination of carboxyl groups (–COO − ) from XG-Ca with Fe sites on the pyrite surface; and (2) calcium-mediated electrostatic bridging between surface hydroxyl groups (–OH) of pyrite and functional groups in XG-Ca. This study proposes an innovative approach of pre-combining xanthan gum with calcium ions, offering valuable insights for developing efficient and green depressants for Cu-S separation.
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Journal of Materials Chemistry C
·
2012
·Vol. 1
·期 6
·1111-1121
·
IF 0
Junjie Li,Xin Hu,Guoxin Gao,Shujiang Ding,Huayi Li,Lanjun Yang,Zhicheng Zhang
For potential application in high energy storage capacitors with high energy density and low energy loss, three sets of poly(vinylidene fluoride-co-trifluoroethylene-co-chlorotrifluoroethylene) [P(VDF-TrFE-CTFE)] grafted with poly(methacrylic ester)s, including poly(methyl methacrylate) (PMMA), poly(ethyl methacrylate) (PEMA) and poly(butyl methacrylate) (PBMA) copolymers, are designed and investigated carefully. Due to their intermediate polarity, relatively high glass transition temperature, and excellent compatibility with PVDF chains, the poly(methacrylic ester) segments introduced could not only dramatically weaken the coupling interactions of oriented polar crystals, but could also accelerate the reversal switching of polar crystal domains along the applied electric field, which leads to well hindered remnant polarization. As a result, the displacement–electric field (D–E) hysteresis behaviors of the graft copolymers could be tuned from typical ferroelectric to either antiferroelectric or linear shape under high electric field. Meanwhile, significantly reduced energy loss and effectively improved energy discharging efficiency were obtained. Compared with PMMA and PBMA, PEMA with intermediate polarity and grafting length exhibits more suitable confinement of the F–P transition of P(VDF-TrFE-CTFE), and thus more desirable energy storage properties are observed in the resultant copolymers. These findings may help to deeply understand the ferroelectric nature of PVDF based fluoropolymers and design new energy storage capacitor materials with high discharged energy density and low energy loss.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qiang Zhang,Ranxiao Ao,Ruijie Gao,Huaming Yang
Transition metals with 3d unoccupied orbitals have superior catalytic activity, but inherent high spin suppresses their adsorption capability, leading to sluggish polysulfide conversion kinetics for Li–S batteries. Herein, we provide Fe–O–Si bridge bonds to manipulate eg filling and induce a high-to-medium spin transition of Fe3+ sites, which enhances polysulfide adsorption and facilitates sulfur redox reaction kinetics. The resultant cathodes exhibit outstanding performances under high sulfur loading, which can deliver a high battery specific energy of 1061 mA h·g–1 even after 100 cycles in Li–S pouch batteries. This work provides new insights into the kinetic and multi-step conversion mechanism of the sulfur redox reaction process, helping in the understanding and design of spin-dependent catalysts.
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高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Ying Xu,Dong Wang,Xin Wang,Jian Dong
The rapid growth of natural gas clathrate hydrate has been a significant safety hazard in off-shore natural gas drilling and gas transport. Alleviation of hydrate formation can be achieved by applying low-dosage hydrate inhibitors of polymers during operation. In order to combine the advantages of high adsorption potential and environmental friendliness, we study the kinetics of hydrate inhibition of amphiphilic highly branched poly(l-lysine) (PLL) by NMR relaxometry. The introduction of n-butyl and cyclohexyl groups in PLLs was found to be significantly effective in prolonging the induction times of sII clathrate hydrates. Key physical–chemical factors involved in the mechanism previously proposed by molecular dynamics simulations can be clarified by NMR relaxometry. Induction times for the formation of hydrate are associated with the interfacial water amount but are not related to the hydrogen bonding strength or dynamics of the free water component. The amphiphilic PLLs in the interface interact with the hydrate surfaces through their hydration shell. Analysis of the molecular motion and freezing kinetics of water in the fluid before and during hydrate formation reveals that the polymers can reduce the rates of hydrate growth from the free water by a factor of 5 to 10. A further significant decrease in the growth rates from small hydrate particles by a factor of 10 to 2600 was observed in the presence of the amphiphilic PLLs with n-butyl and cyclohexyl groups. The distinct crystal growth kinetics in the heterogeneous interface are influenced by the terminal alkyl groups of the polymers, with changing growth geometry or crystal shapes and consistent with the interfacial Gibbs–Thomson effect. A high Avrami index value of the isothermal crystal growth and nonfreezable water amount favors a long induction time. The PLL inhibitors adsorb to the hydrate surface and act via an interfacial mechanism.
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