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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

High-efficiency ammonia electrosynthesis on self-supported Co2AlO4 nanoarray in neutral media by selective reduction of nitrate

Zhiqin Deng,Jie Liang,Qian Liu,Chaoqun Ma,Lisi Xie,Luchao Yue,Yuchun Ren,Tingshuai Li,Yongsong Luo,Na Li,Bo Tang,Abdulmohsen Ali Alshehri,Imran Shakir,Philips O. Agboola,Shihai Yan,Baozhan Zheng,Juan Du,Qingquan Kong,Xuping Sun

A Co 2 AlO 4 nanosheet array on carbon cloth (Co 2 AlO 4 /CC) is proposed as a superb electrocatalyst for converting nitrate (NO 3 − ) to ammonia (NH 3 ). In 0.1 M PBS solution with 0.1 M NO 3 − , it attains an NH 3 yield of 7.9 mg h −1 cm −2 with a Faradaic efficiency of 92.6%, with high durability. A Zn-NO 3 − battery with such Co 2 AlO 4 /CC as cathode offers a power density of 3.43 mW cm −2 with an NH 3 yield of 750 μg h −1 cm −2 . Theoretical calculations reveal that Al ions reduce the electron cloud density on the surface of Co, making it highly conducive to NO 3 − adsorption at Co sites. Additionally, Co 2 AlO 4 (2   2   0) surface inhibits hydrogen evolution reaction but is highly active for NO 3 − reduction with a low energetically uphill pathway (ΔG of 0.42 eV) for the potential-determining step (*NO 3 to *NO 3 H), much smaller than that of Co 3 O 4 (2   2   0) (ΔG of 0.83 eV).

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TALANTA · 2022 · IF 6.556

Monomer-mediated fabrication of microporous organic network@silica microsphere for reversed-phase/hydrophilic interaction mixed-mode chromatography

Hao-Fei Sun,Yuan-Yuan Cui,Chang-Qing Zhen,Cheng-Xiong Yang

Microporous organic networks (MONs) are promising in high performance liquid chromatography (HPLC) with large specific surface area, good hydrophobicity and stability. However, their superhydrophobic structures restrict MONs-based HPLC only in reversed-phase mode. To decrease the hydrophobicity of pristine MONs and to expand their broad application in HPLC, here we described the monomer-mediated fabrication of core-shell MON-2COOH@SiO 2 microspheres for reversed-phase liquid chromatography (RPLC)/hydrophilic interaction liquid chromatography (HILIC) mixed-mode chromatography for the first time. The –COOH groups were introduced into MONs’ skeleton to improve their hydrophilicity and to provide hydrophilic interaction sites. The MON-2COOH was grafted onto silica via a monomer mediated method to produce monodispersed core-shell microspheres. By adjusting the concentration of reactants, the thickness of MON-2COOH shell was easily manipulated. The packed MON-2COOH@SiO 2 column showed high resolution and selectivity for separating both hydrophobic (alkylbenzenes, polycyclic aromatic hydrocarbons , anilines and phenols) and hydrophilic (nucleoside and nucleic bases) probes, highlighting the promise of MONs in mixed-mode HPLC. The MON-2COOH@SiO 2 column also achieved good separation to sulfonamides, nonsteroidal anti-inflammatory drugs, flavonoids and phenylurea herbicides , and offered better resolution than commercial C18 and pristine SiO 2 column. Multiple retention mechanisms were also found on MON-2COOH@SiO 2 packed column, underlining the great potential of MONs in mixed-mode HPLC.

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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 32 ·16883-16890 · IF 14.511

Interface coupling induced built-in electric fields boost electrochemical nitrate reduction to ammonia over CuO@MnO2 core–shell hierarchical nanoarrays

You Xu,Youwei Sheng,Mingzhen Wang,Tianlun Ren,Keke Shi,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang

Electrochemical nitrate reduction to ammonia emerges as an attractive and promising technology for nitrate removal from water and simultaneous ammonia electrosynthesis, which demands electrocatalysts with high activity and selectivity. Herein, we designed CuO@MnO2 1D core–2D shell hierarchical nanoarrays supported on a copper foam substrate (CuO@MnO2/CF) for electrocatalytic nitrate-to-ammonia conversion. The decoration of CuO 1D nanowire arrays with MnO2 2D nanosheets brings about abundant exposed active sites and facilitates mass transfer. More importantly, the CuO/MnO2 heterogeneous nanointerface affords a well-designed built-in electric field in the interface region, which could trigger interfacial accumulation of nitrate ions and accelerate nitrate electroreduction kinetics by optimizing the chemisorption of nitrate ions or/and reaction intermediates. With these properties, an impressive electrocatalytic nitrate-to-ammonia capability was achieve over CuO@MnO2/CF (nitrate conversion: 99.38%, ammonia faradaic efficiency: 94.92%, and ammonia selectivity: 96.67%). This study opens new avenues for the rational construction of efficient electrocatalysts for nitrate removal and ammonia electrosynthesis.

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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Synergism of Interfaces and Defects: Cu/Oxygen Vacancy-Rich Cu-Mn3O4 Heterostructured Ultrathin Nanosheet Arrays for Selective Nitrate Electroreduction to Ammonia

Hongjing Wang,Qiqi Mao,Tianlun Ren,Tongqing Zhou,Kai Deng,Ziqiang Wang,Xiaonian Li,You Xu,Liang Wang

Achieving high efficiency in nitrate (NO3–) to ammonia (NH3) electrocatalysis requires the exploration of advanced electrocatalysts with a well-designed composition and architecture. In this work, a facile one-step hydrothermal approach was developed for the construction of novel Cu/oxygen vacancy-rich Cu-Mn3O4 heterostructured ultrathin nanosheet arrays on Cu foam (Cu/Cu-Mn3O4 NSAs/CF). Two-dimensional ultrathin nanosheet arrays could increase the exposure of catalytically active centers, and the heterogeneous nanointerface and oxygen vacancies synergistically improve the nitrate-to-ammonia activity over the active centers. Due to the desirable compositional and structural advantages, the Cu/Cu-Mn3O4 NSAs/CF demonstrated excellent performance for the electrocatalytic nitrate reduction to ammonia with high ammonia selectivity (87.6%) and Faradic efficiency (92.4%).

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ENVIRONMENTAL POLLUTION · 2021 · IF 8.071

Selective production of singlet oxygen from zinc-etching hierarchically porous biochar for sulfamethoxazole degradation

Chen Sun,Tong Chen,Qunxing Huang,Xiaoguang Duan,Mingxiu Zhan,Longjie Ji,Xiaodong Li,Jianhua Yan

Porous carbons are appealing low-cost and metal-free catalysts in persulfate-based advanced oxidation processes . In this study, a family of porous biochar catalysts (ZnBC) with different porous structures and surface functionalities are synthesized using a chemical activation agent (ZnCl 2 ). The functional biochars are used to activate persulfate for sulfamethoxazole (SMX) degradation. ZnBC-3 with the highest content of ketonic group (C O, 1.25 at%) exhibits the best oxidation efficiency, attaining a rate constant ( k obs ) of 0.025 min −1 . The correlation coefficient of the density of C O to k obs ( R 2  = 0.992) is much higher than the linearity of the organic adsorption capacity to k obs ( R 2  = 0.694), implying that C O is the intrinsic active site for persulfate activation. Moreover, the volume of mesopore ( R 2  = 0.987), and Zeta potential ( R 2  = 0.976) are also positive factors in PS adsorption and catalysis. In the mechanistic study, we identified that singlet oxygen is the primary reactive oxygen species . It can attack the –NH 2 group aligned to the benzene ring to form dimer products which could be adsorbed on the biochar surface to reach complete removal of the SMX. The optimal pH range is 4–6 which will minimize the electrostatic repulsion between ZnBCs and the reactants. The SMX degradation in ZnBC/PS system was immune to inorganic anions but would compete with organic impurities in the real wastewater . Finally, the biochar catalysts are filled in hydrogel beads and packed in a flow-through packed-bed column. The continuous system yields a high removal efficiency of over 86% for 8 h without decline, this work provided a simple biochar-based persulfate catalyst for complete antibiotics removal in salty conditions.

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Advanced Materials Interfaces · 2021 ·Vol. 8 ·期 19 ·2100588 · IF 6.147

Internal–External Stabilization Strategies Enable Ultrastable and Highly Luminescent CsPbBr3 Perovskite Nanocrystals for Aqueous Fe3+ Detection and Information Encryption

Jie Guan,Ying-zhuo Shen,Yun Shu,Dangqin Jin,Qin Xu,Xiao-Ya Hu

The high photoluminescence quantum yield (PLQY) of perovskite nanocrystals (PNCs) makes them promising candidates in optoelectronics. However, the easy loss of structural integrity and fast chemical degradation upon exposure to moisture influence their reliable applications in aqueous solutions. Here, a hierarchical surface construction strategy is rationally designed to fulfill an internal–external stabilization of PNCs. Carbon quantum dots (CQDs) and cetyltrimethyl ammonium bromide (CTAB) have been demonstrated stabilized PNCs internally by eliminating the proton transfer-induced ligand desorption. Meanwhile, CTAB acts as a cationic surfactant in consolidating the subsequent SiO 2 coating to prevent the PNCs from external environments. Based on the resulted PNCs, a sensitive and selective fluorescence film sensor for Fe 3+ detection is successfully constructed. The fluorescence of PNCs at 525 nm is quenched after the addition of Fe 3+ in the concentration range from 770 p m to 411 µ m . As Fe 3+ ions attached to the surface of the film are removed with water, the fluorescence of the film can be easily recovered. Owing to this character, the application of the PNCs toward the confidential information encryption has been proved. This work provides an effective design strategy to improve the stability of PNCs and extends their applications in sensing and encryption areas.

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Journal of Functional Foods · 2021 · IF 4.451

Potential in vitro anti-neuroinflammatory sterols from mango fruits (Mangifera indica L.)

Liangmiao Luo,Yi Wang,Yihai Wang,Jingwen Xu,Xiangjiu He

Mango is one of the most popular fruit in tropical and subtropical regions of the world. In this study, previously undescribed two sterols ( 1 – 2 ) and one terpenoid ( 10 ), as well as ten known phytochemicals ( 3 – 9 , 11 – 13 ), were isolated and identified from mango fruits. In vitro anti-neuroinflammatory activity of the purified compounds was evaluated and most of them exhibited pronounced bioactivity. Among them, compounds 2 and 5 exhibited the most significant anti-neuroinflammatory effects, which were comparable to that of indomethacin (positive control) and suggested that the sterols in the fruits of mango played important roles for the anti-neuroinflammatory activity. Further, Western blotting, quantitative PCR and immunofluorescence staining assays were performed to confirm that compounds 2 and 5 exerted the anti-neuroinflammatory through the NF-κB pathway. The study provided a phytochemical evidence for further development and utilization of the fruits of mango in health products.

CAS / MDL: 1465-25-4 63-74-1
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Facet-controlled palladium nanocrystalline for enhanced nitrate reduction towards ammonia

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

A novel CNTs-Fe3O4 synthetized via a ball-milling strategy as efficient fenton-like catalyst for degradation of sulfonamides

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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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 30 ·16411-16417 · IF 12.732

Atomic defects in pothole-rich two-dimensional copper nanoplates triggering enhanced electrocatalytic selective nitrate-to-ammonia transformation

You Xu,Mingzhen Wang,Kaili Ren,Tianlun Ren,Mengying Liu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang

The development of efficient catalysts for electrocatalytic selective conversion of nitrate pollutants into valuable ammonia is a project of far-reaching importance. This work demonstrated the in situ electroreduction of pre-synthesized CuO nanoplates into defect-rich metallic Cu nanoplates and evaluated their electrocatalytic nitrate-to-ammonia activity. Concentrated atomic defects in the as-converted Cu nanoplates could favor the adsorption, enrichment and confinement of nitrate ions and pivotal reaction intermediates, selectively promoting eight-electron reduction (NH3 formation). Consequently, the resultant defect-rich Cu nanoplates exhibit a significant ammonia production rate of 781.25 μg h−1 mg−1, together with excellent nitrate conversion (93.26%), high ammonia selectivity (81.99%) and good electrocatalytic stability, superior to the defect-free Cu nanoplate counterpart. Isotope labelling experiments demonstrated that the source of ammonia was from nitrate. Both 1H NMR and colorimetric methods were used to quantify the ammonia yield.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2020 · IF 5.162

Characterization and immunological activity of polysaccharides from Potentilla chinensis

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.

CAS / MDL: 1465-25-4 63-74-1
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Drug Testing and Analysis · 2020 ·Vol. 13 ·期 3 ·720-728 · IF 2.903

New qualitative analysis strategy for illicit drugs using Raman spectroscopy and characteristic peaks method

Cui-Mei Liu,Hong-Yuan He,Lin Xu,Zhen-Dong Hua

Performing fast qualitative identification of seized illegal drugs by Raman spectroscopy is challenging due to fluorescence interference as well as chemical complexity. Spectrometers with 785-nm excitation, 1,064-nm excitation, and sequentially shifted excitation (SSE) were compared for their effect on fluorescence reduction. The characteristic peaks method, which is independent of cutting agents, was tested as a new strategy to broaden the application of the Raman technique. The suitability of the characteristic peaks method was fully examined by analyzing a large amount of seized illegal drugs, including 72 methamphetamine hydrochloride (concentration range of 13.9%–99.4%), 68 ketamine hydrochloride (17.7%–99.8%), 176 heroin hydrochloride (5.2%–79.5%), 51 cocaine hydrochloride (21.1%–94.5%), and 33 cocaine base (30.9%–92.5%) samples. The results showed that seized methamphetamine, ketamine, and cocaine samples had no or little fluorescence. Hence, in regard to detection of these samples, the advantage of using 1,064-nm excitation and SSE compared with 785-nm excitation was quite limited. Regarding the heroin samples, a significant improvement of the “high” confident positive detected rate was evident for 1,064 nm excitation (60.8%) and SSE (61.4%), compared with 785-nm excitation (13.1%). However, it was also seen that even if 1,064-nm excitation and SSE were applied, the fluorescence of heroin samples was still unable to be fully overcome. By using the characteristic peaks method, low LOD results of 5%–20% were acquired for 40 types of drug mixtures, and lower LODs were obtained for the 60% of the drug mixtures compared with library searching method. Raman spectroscopy in conjunction with the characteristic peaks method was shown to be fast, simple, accurate, and sensitive in the qualitative analysis of seized drug samples.

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