Nature Communications
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2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Zhang Rong,Li Chuan,Cui Huilin,Wang Yanbo,Zhang Shaoce,Li Pei,Hou Yue,Guo Ying,Liang Guojin,Huang Zhaodong,Peng Chao,Zhi Chunyi
Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of nitrate reduction under acidic conditions is rarely reported. In this work, we demonstrate the potential of TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity for selective and rapid nitrate reduction to ammonia under acidic conditions. Hybridized with iron phthalocyanine, the resulting catalyst displays remarkably improved efficiency toward ammonia formation owing to the enhanced nitrate adsorption, suppressed hydrogen evolution and lowered energy barrier for the rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed with high open-circuit voltage of 1.99 V and power density of 91.4 mW cm –2 . Further, the environmental sulfur recovery can be powered by above hybrid battery and the hydrazine-nitrate fuel cell can be developed for simultaneously hydrazine/nitrate conversion and electricity generation. This work demonstrates the attractive potential of acidic nitrate reduction for ammonia electrosynthesis and broadens the field of energy conversion.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2023
·Vol. 332
·期 12
·5059-5070
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IF 1.6
Guo Zifang,Zhang Yang,Jiao Limin,Li Yifan,Lin Zijian,Du Xiangyi,Zhao Xing,Gao Xuan,Yu Guobing,Liu Chunyu,Lin Mingzhang
The radiolytic behaviors of aqueous ammonia solutions under γ-ray irradiation were investigated, focusing on several factors, including initial ammonia concentration, absorbed dose, and H 3 BO 3 concentration. The main species including ammonia, H 2 O 2 , nitrogen oxides, and H 2 , were quantitatively analyzed. The results revealed the significant influence of the initial ammonia concentration on the radiolytic behavior of the aqueous ammonia solution. The existence of ammonia in the solution exhibited suppression of the concentrations of H 2 O 2 and O 2 . Furthermore, the radiolysis of aerated aqueous ammonia solution led to the formation of nitrogen oxides (NO 2 − and NO 3 − ). This process was driven by multiple oxidation reactions, in which O 2 and ·OH played crucial roles. Interestingly, the addition of H 3 BO 3 provided protection to ammonia during γ irradiation, while the concentration of H 2 O 2 was increased.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xia Zhan,Rui Ge,Teng Huo,Juan Lu,Jiding Li
Graphene oxide (GO) membranes exhibit ultrafast water permeation properties, which have been employed in various membrane-based separations including nanofiltration for dye removal from textile wastewater. However, it’s still a great challenge to achieve precise control over the microstructure of GO membranes and obtain ultrathin GO membranes with exceptional separation efficiency and robust membrane structure. Herein, in-situ confined interfacial polymerization (IP) is proposed for fabricating loose polyamide (PA)@GO hybrid membranes with high permeance and dye rejection as well as robust membrane stability. A new diamine of sulfadiazine (SA) with intrinsic hydrophilic and conjugated sulfonamide groups is employed as cross-linker of GO membranes and monomer of PA in IP process, simultaneously. PA is in-situ synthesized in confined GO interlayer via IP process and intercalated into GO interlayer, which enlarges the interlayer spacing of GO membranes gradiently. The combination of hydrophilic PA nanofiltration layer on GO membrane surface and the PA intercalated GO membrane with varying interlayer spacing creates hierarchical transport channels for water molecules, which contributes to the high water permeance. Moreover, the less reactive SA monomer endows PA@GO selective layer with appropriate negative charge and loose transport channels, which contributes to both of high permeance and dye rejection due to Donnon effect and size exclusion effect. The PA@GO hybrid membrane exhibits high permeance of 75.5 L/(m 2 ·h·bar) with TB dye rejection of 99.8 %, and exhibits low NaCl rejection of 11.6 %. Moreover, PA@GO hybrid membrane shows good fouling resistance and long-term stability as well as stable separation performance under harsh conditions. Both of high permeance and dye rejection of PA@GO hybrid membrane suggests that the integration of PA nanofiltration layer and GO membrane via in-situ confined interfacial polymerization can achieve the delicate control over the interlayer channel structure and the physicochemical properties of the membrane surface of GO membranes, which offers a promising method to break through the trade-off effect between permeability and selectivity of GO membranes.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
·
IF 8.4
Shuai Liu,Hao Qu,Lili Yao,Yu Mao,Ling Yan,Baolei Dong,Lei Zheng
Rapid and accurate nitrite ions (NO 2 − ) detection is necessary to ensure food safety. Herein, a new portable method for detecting NO 2 − using hydrogel microspheres is proposed. Specifically, N-(1-naphthyl) ethylenediamine (NED) was immobilized on sodium alginate (SA) to obtain the SA-NED conjugate via covalent linking. The SA-NED microspheres were prepared in a Ca 2+ solution using an extrusion strategy based on the strong chelation between SA and Ca 2+ . The SA-NED microspheres exhibited superior adsorption capacity for NO 2 − , which agrees with the Langmuir isotherm model. Then, based on the Griess reaction , a microsphere-based colorimetric sensor was developed for rapid, quantitative, and on-site NO 2 − detection via a smartphone-based sensing platform. The entire detection procedure can be completed within 35 min. The microsphere-based sensor exhibited a detection limit of 0.02 μg mL –1 with recoveries ranging from 89.7% to 104.8% in different food samples. Moreover, the microsphere-based sensor showed good tolerance to the complex food matrix. Water and milk samples could be directly measured without pretreatment , and pickles and sausages only required simple homogenization before measurements. Our study provides an effective approach for rapid and on-site monitoring of NO 2 − .
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Dongsheng Lu,Tiesen Liu,Jinyu Han,Jiankang Zhao,Hua Wang
Electroreduction of nitrate to ammonia, a potential route for producing ammonia, is still confronted with a great challenge on developing efficient electrocatalysts. In this work, a reduced yolk-shell Co-based oxides (R-Co 3 O 4 ) electrocatalyst with oxygen vacancy-rich Co 3 O 4 and CoO was designed for nitrate reduction . This catalyst presented a nearly 100 % Faradaic efficiency (FE) of ammonia in a low potential from −0.05 to −0.1 V vs. RHE, and a maximum ammonia production rate of 7.25 mg h −1 mg cat. -1 at −0.05 V vs. RHE in 0.1 M KOH + 1000 ppm KNO 3 electrolyte. X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) pattern proved that the content of Co 2+ was dramatically increased in R-Co 3 O 4 . The kinetic correlation experiments and Operando Raman spectra preliminarily manifest that the potential limiting step is the reduction of adsorbed *NO 3 . The density functional theory (DFT) calculations consistently demonstrated that on both oxygen-rich Co 3 O 4 and CoO, the adsorption of key intermediates (*NO 3 , *NO and *NH) are greatly enhanced on the bridge site between two Co 2+ , boosting the nitrate reduction at low over-potential. This work is helpful to design the catalytic material with rich and low-valence sites towards electroreduction of nitrate to ammonia.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 43
·e2311585120
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IF 11.1
Chao-Hai Gu,Song Wang,Ai-Yong Zhang,Chang Liu,Jun Jiang,Han-Qing Yu
Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure–performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure–reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.
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INORGANIC CHEMISTRY
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2023
·
IF 4.6
Zuan Yu,Jiangwei Xie,Tianlun Ren,Hongjie Yu,Kai Deng,Ziqiang Wang,Hongjing Wang,Liang Wang,You Xu
Utilizing nitrate from wastewater as a N-source for ammonia synthesis via electrocatalysis is of significance for both environmental protection and ecological nitrogen cycle balance, which requires high-performance electrocatalysts to drive selective nitrate-to-ammonia transformation. In this work, an electrochemical postmodification strategy was developed to regulate the surface structure of presynthesized Cu nanodendrites at the atomic level. A combination of physicochemical characterization and electrochemical study demonstrates that such a treatment could induce surface Cu atom rearrangement and result in increased electrochemically active surface area and high density of surface-active sites, disclosing a high electrocatalytic nitrate-to-ammonia capability, with an optimal NH3 yield rate of 0.2238 mmol h–1 cm–2 and a corresponding Faradaic efficiency of 94.43%. This study may provide a guiding design avenue for atomic arrangement engineering of metallic nanocrystals via electrochemical postmodification for nitrate reduction reaction and other energy conversion electrocatalysis.
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FOOD CHEMISTRY
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2021
·
IF 7.514
Murtaza Ali,Jun-Hu Cheng,Da-Wen Sun
This study investigated the effect of plasma-activated liquid (PAL) including plasma-activated water (PAW) and plasma-activated buffer solution (PABS) for the reduction of chlorothalonil (CTL) and thiram (THM) pesticide residues on tomato fruit. Results revealed that the PAL obtained by using atmospheric air as the feed gas, CTL residues were decreased to 85.3% and 74.2% and THM residues decreased to 79.47 and 72.21% after treatments with PAW 10 and PABS 10 , respectively, and increasing the activation time caused a significant reduction in fungicide residues. In addition, CTL and THM residues were also decreased while increasing the activation time of PAL using Ar/O 2 as the feed gas, the concentrations of the CTL residues were decreased to 75.07 and 69.89% for PAW 10 and PABS 10 , respectively and THM residues decreased to 65.89 and 61.91% for PAW 10 and PABS 10 , respectively. Oxidation-reduction potential (ORP) and electrical conductivity (EC) were increased significantly after plasma treatment, while pH values of both solutions were decreased significantly with activation time. NO 3 − and NO 2 − concentrations of PAW increased significantly, while for PABS, NO 3 − concentration decreased but NO 2 − , with increasing the plasma activation time. Additionally, washing with PAW and PABS caused no notable negative impact on tomato fruit. Results confirmed that PAL treatments showed a significant reduction of CTL and THM fungicide residues ( p < 0.05) in tomato without affecting the quality.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Yi Han,Xinyi Zhang,Wenwen Cai,Huan Zhao,Yanyun Zhang,Yuyao Sun,Zhiqiang Hu,Shaoxiang Li,Jianping Lai,Lei Wang
Electrochemical nitrate reduction reaction (NO 3 − RR) is considered an appealing way for producing ammonia (NH 3 ) under ambient conditions and solving environmental problems caused by nitrate, whereas the lack of adequate catalysts hampers the development of NO 3 − RR. Here, we firstly demonstrate that the Pd nanocrystalline with a well-desired facet can act as a highly efficient NO 3 − RR electrocatalyst for ambient ammonia synthesis. Pd (1 1 1) exhibits excellent activity and selectivity in reducing NO 3 − to NH 4 + with a Faradaic efficiency of 79.91% and an NH 4 + production of 0.5485 mmol h −1 cm −2 (2.74 mmol h −1 mg −1 ) in 0.1 M Na 2 SO 4 (containing 0.1 M NO 3 − ), which is 1.4 times higher than Pd (1 0 0) and 1.9 times higher than Pd (1 1 0), respectively. Density functional theory (DFT) calculation reveals that the superior NO 3 − RR activity of Pd (1 1 1) originates from its optimized activity of NO 3 − adsorption, smaller free energy change of the rate-limiting step (*NH 3 to NH 3 ), and poorer hydrogen evolution reaction activity (HER, competitive reaction). This work not only highlights the potentials of Pd-based nanocatalysts for NO 3 − RR but also provides new insight for the applications in NO 3 − RR of other facet-orientation nanomaterials.
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CHEMOSPHERE
·
2021
·
IF 7.086
Yunbo Liu,Xuemei Zhang,Jinhua Deng,Yong Liu
A novel composite (CNTs-Fe 3 O 4 ) was synthesized by a ball-milling strategy and characterized by BET, SEM, FTIR , XRD and VSM. The as-fabricated CNTs-Fe 3 O 4 was used to remove six sulfonamides by a Fenton degradation process, including sulfanilamide (SAM), sulfamerazine (SMR), sulfadimethoxine (SMX), sulfadiazine (SDZ), sulfamethazine (SMT) and sulfametoxydiazine (SMD). The degradation behaviors of six sulfonamides in CNTs-Fe 3 O 4 /H 2 O 2 system and the relationship between molecular structure of sulfonamides and their degradation behaviors were investigated systematically. Batch experimental results showed that the as-fabricated CNTs-Fe 3 O 4 had excellent Fenton catalytic activity for the degradation of sulfonamides due to its unique porous structure and the good combination mode of CNTs with Fe 3 O 4 particles. The first-order kinetic mode could better describe the degradation behaviors of six sulfonamides in CNTs-Fe 3 O 4 /H 2 O 2 system, and the degradation rate constant could be ordered as: SAM < SMT < SDZ < SMR < SMD < SMX. The quantitative relationship between the Mulliken charge of sulfonamides (x) and their degradation rate constant (y) in CNTs-Fe 3 O 4 /H 2 O 2 system could be described as: y = - 28.719x + 15.67 (R 2 = 0.957). Finally, the possible synthesis mechanisms of CNTs-Fe 3 O 4 and the degradation mechanisms of sulfonamides in CNTs-Fe 3 O 4 /H 2 O 2 system was proposed.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
·
IF 5.162
Yuanhao Qiu,Zahra Batool,Rui Liu,Guoqing Sui,Bulei Sheng,Xinhua Zheng,Dan Xu
Three novel polysaccharides (PCPW, PCPS1 and PCPS2) were isolated from Potentilla chinensis and subjected to structural analysis by using spectral and physicochemical methods. The molecular weights of PCPW, PCPS1 and PCPS2 were calculated to be 4.45 × 10 3 Da, 1.18 × 10 4 Da and 4.23 × 10 4 Da, respectively. Analysis of monosaccharides composition confirmed that PCPW was composed of mannose, rhamnose, glucose, galactose and arabinose, while the two acidic polysaccharides PCPS1 and PCPS2 were consisted of six monosaccharides, including mannose, rhamnose, galacturonic acid, glucose, galactose and arabinose respectively. In addition, the main linkages of glycosidic bonds of PCPS2 were 1, 4-linked-rha, 1, 4-linked-man,1, 4-linked-galA and 1, 6-linked-man. Immunological tests indicated that both PCPW and PCPS2 could increase NO production of RAW264.7 cells, and promote splenocyte proliferation. All three polysaccharides proved to be activators of NF-κB. Overall, three polysaccharides showed a good immunological activity and pose great potential as a novel food or drug additive.
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ENVIRONMENTAL POLLUTION
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2020
·
IF 6.793
Yuanyuan Peng,Wenhua Tong,Yi Xie,Wanrong Hu,Yonghong Li,Yongkui Zhang,Yabo Wang
Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation have attracted increasing attention in recent years for organic pollutants removal . Herein, we put forward a facile method to form cobalt phosphide/carbon composite for PMS activation. Combining impregnation approach with pyrolysis treatment enabled the formation of Co 2 P/biochar composites using baker’s yeast and Co 2+ as precursors. The as-synthesized products exhibited excellent catalytic activity for sulfamethoxazole (SMX) degradation over the pH range 3.0–9.0 b y activating PMS. For example, 100% of SMX (20 mg L −1 ) removal was achieved in 20 min with catalyst dosage of 0.4 g L −1 and PMS loading of 0.4 g L −1 . Near zero Co 2+ leaching was observed during catalytic reaction, which remarkably lowered the toxic risk of transition metal ion in water. Meanwhile, the reusability of catalyst could be attained by thermal treatment. SMX degradation intermediates were identified by liquid chromatography-mass spectrometry (LC-MS), which facilitated the proposal of possible SMX degradation pathways. Ecological Structure Activity Relationships (ECOSAR) analysis indicated that SMX degradation intermediates may not pose ecological toxicity to the environment. Further investigation verified that Co 2 P/biochar composites could set off PMS activation not only for the degradation of SMX but also for other sulfonamides. In this study, we not only developed a facile method of utilizing environmental-benign biomass for transition metal phosphide/carbon composite formation, but also achieved highly efficient antibiotic elimination by PMS-based AOP.
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