Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Luo Haolin,Liu Zhixi,Lv Haifeng,Vequizo Junie Jhon M.,Zheng Mengting,Han Feng,Ye Zhen,Yamakata Akira,Shangguan Wenfeng,Lee Adam F.,Wu Xiaojun,Kazunari Domen,Lu Jun,Jiang Zhi
N-type sulfide semiconductors are promising photocatalysts due to their broad visible-light absorption, facile synthesis and chemical diversity. However, photocorrosion and limited electron transport in one-step excitation and solid-state Z-scheme systems hinder efficient overall water splitting. Liquid-phase Z-schemes offer a viable alternative, but sluggish mediator kinetics and interfacial side reactions impede their construction. Here we report a stable Z-scheme system integrating n-type CdS and BiVO₄ with a [Fe(CN)₆]³⁻/[Fe(CN)₆]⁴⁻ mediator, achieving 10.2% apparent quantum yield at 450 nm with stoichiometric H₂/O₂ evolution. High activity reflects synergies between Pt@CrO x and Co 3 O 4 cocatalysts on CdS, and cobalt-directed facet asymmetry in BiVO₄, resulting in matched kinetics for hydrogen and oxygen evolution in a reversible mediator solution. Stability is dramatically improved through coating CdS and BiVO 4 with different oxides to inhibit Fe 4 [Fe(CN) 6 ] 3 precipitation and deactivation by a hitherto unrecognized mechanism. Separate hydrogen and oxygen production is also demonstrated in a two-compartment reactor under visible light and ambient conditions. This work unlocks the long-sought potential of n-type sulfides for efficient, durable and safe solar-driven hydrogen production.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Xiaoqin Wang,Wenqing Li,Zhenhua Li,Tianjiao Han,Jinqiao Rong,Jiangbo Fan,Linjuan Huang,Yu Lu,Zhongfu Wang
Human milk glycans are complex carbohydrates , which play a pivotal role in infant health and neonatal development . Maternal secretor status is known to affect free oligosaccharides in milk. Here, the milk N -glycome of secretor (Se+) and nonsecretor (Se−) individuals was qualitatively and quantitatively analyzed by hydrophilic interaction chromatography-electrospray ionization-tandem mass spectrometry. The total glycosylation , fucosylation , and sialylation of N -glycans was three times higher in the Se+ group compared to the Se− group ( p < 0.001) per equal volume of milk. Importantly, 52 out of 63 N -glycans—including the eight most abundant ones—differed greatly between Se+ and Se− individuals ( p < 0.05). Moreover, nine N -glycans (H5N3F1, H6N3, H3N5F1, H5N5F1, H5N5F1S1, H5N4F3S1, H6N4F2S1, H6N5F4S1, and H8N7S1) were >10 times more abundant in Se+ milk than in Se− milk. These findings lay a glycomics-basis for designing personalized nutrition supplements for infants.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Chao Li,Yun Teng,Huanong Cheng,Hongwei Jin,Kangkang Li,Zhou Feng,Zhonghao Li,Xinshun Tan,Shiqing Zheng
The density and viscosity of N-butylmorpholine bromide iron-based ionic liquids ( r FeCl 3 / [Nbmm]Br) with two iron-morpholine ratios ( r = 0.8 and 1.0) mol·mol −1 were measured at 303.15–348.15 K and 101.3 kPa. Density and viscosity data were fitted by empirical correlations for temperature. The average relative errors were less than 0.02 % and 2 %, respectively. The density and viscosity decrease with increasing temperature. The density increases with the increase of r , while the viscosity shows the opposite trend. The gas-liquid equilibrium data of H 2 S in r FeCl 3 /[Nbmm]Br were measured by the isochoric pressure drop method at temperatures of 303.15–348.15 K, pressures of 0–200 kPa, and r of 0.8 and 1.0 mol·mol −1 . The total solubility of H 2 S increases with decreasing temperature, increasing pressure, and decreasing r . The measured solubility data were fitted by the reaction equilibrium thermodynamic model. Chemical reaction equilibrium constant and the Henry's constant at different temperatures and different r were obtained. The average relative error of model fitting is less than 3 %. The results show that the chemical reaction equilibrium constant and the Henry’s constant both decrease with the increase of r , and decrease of temperature. Effect of molecular structure on reaction equilibrium constants was explained by quantum chemistry calculation. The absorption of H 2 S in r FeCl 3 / [Nbmm]Br at low pressure is dominated by chemical absorption. With the increase of pressure, the proportion of physical absorption continues to increase, and gradually occupies the main part.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 15
·6643-6655
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IF 4.5
Zhang Hengchao,Li Yarou,Zhang Yupan,Wu Junfeng,Hu Jiandong,Li Shixin,Li Lanlan
Heavy metal pollution in the environment has posed a serious threat to human health and ecosystems. Therefore, it is urgent to develop a fast and effective sensing method for detecting heavy metal ions (HMIs). A simple and rapid ultrasonic mixing method was used to prepare nanocomposites consisting of cysteine, multi-walled carbon nanotubes, and nitrogen-doped molybdenum disulfide (L-Cys/MWCNTs/N-MoS 2 ). Fully combining the excellent features of 2D materials and carbon nanomaterials, the nanocomposites have been successfully used as sensor interface materials for the simultaneous detection of lead ions (Pb 2+ ) and cadmium ions (Cd 2+ ). The L-Cys/MWCNTs/N-MoS 2 @GCE sensor has a wide linear range for the detection of Pb 2+ and Cd 2+ , with the detection limits as low as 0.67 nM and 5.3 nM, respectively. In addition, the sensor performs well in stability, reproducibility, and anti-interference performance. The L-Cys/MWCNTs/N-MoS 2 @GCE sensor can also be used for the detection of Pb 2+ and Cd 2+ in tap water and lake water with good recovery (> 90%), which may provide a promising strategy for the simultaneous in situ and sensitive detection of heavy metal ions in the aqueous environment.
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MOLECULES
·
2023
·Vol. 28
·期 10
·4136
·
IF 4.6
Yongwang Ren,Huizhong Xu,Beibei Han,Jing Xu
At present, the selective hydrogenation of α, β-unsaturated aldehydes remains a challenge due to competition between unsaturated functional groups (C=C and C=O). In this study, N-doped carbon deposited on silica-supported nickel Mott–Schottky type catalysts (Ni/SiO2@NxC) was prepared for the selective hydrogenation of cinnamaldehyde (CAL) by using the respective hydrothermal method and high-temperature carbonization method. The prepared optimal Ni/SiO2@N7C catalyst achieved 98.9% conversion and 83.1% selectivity for 3-phenylpropionaldehyde (HCAL) in the selective hydrogenation reaction of CAL. By constructing the Mott–Schottky effect, the electron transfer from metallic Ni to N-doped carbon at their contact interface was promoted, and the electron transfer was demonstrated by XPS and UPS. Experimental results indicated that by modulating the electron density of metallic Ni, the catalytic hydrogenation of C=C bonds was preferentially performed to obtain higher HCAL selectivity. Meanwhile, this work also provides an effective way to design electronically adjustable type catalysts for more selective hydrogenation reactions.Keywords:Ni catalyst;N-doped carbon;electronic effect;cinnamaldehyde hydrogenation
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2022
·Vol. 26
·期 7
·e202200489
·
IF 2.551
Wenlin Zhang,Tingting He,Shimeng Liu,Lu-Hua Zhang,Fengshou Yu
Graphical Cobalt phthalocyanine was supported on N-doped MXene via axial coordination and π-π stacking. The formed axial coordination configuration N−Co−N 4 can effectively break the planar structure of Co-N 4 and enhance the oxygen reduction performance with an E 1/2 of 0.863 V, which is better than the 20 wt.% Pt/C catalyst of 0.85 V. The precise control of electronic configurations of catalytic sites via molecular engineering is significantly desirable for boosting electrocatalytic activity. We reported a new-type composite electrocatalyst with cobalt phthalocyanine supported on N-doped MXene nanosheets (N-MXene/CoPc) through a self-assembly process. Beneficial from the joint action of N sites participation and axial coordination, N-MXene/CoPc exhibits a high ORR activity with positive onset potential (E onset =0.98 V vs. RHE) and half-wave potential (E 1/2 =0.863 V), which is superior over the pristine CoPc (E 1/2 =0.72 V) and the composite with undoped MXene as support (MXene/CoPc, E 1/2 =0.771 V). Additionally, N-MXene/CoPc exhibits an excellent durability with only 8.5 % attenuation after 25000 s of continuous i-t test, while a more obvious decay 18.6 % for 20 wt.% Pt/C. This work not merely reported a robust ORR catalyst, but more provides a reasonable design strategy for nonnoble-metal catalysts through catalyst-support interactions.
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CLINICA CHIMICA ACTA
·
2022
·
IF 6.314
Jiyun Zhang,Zhizhen Lai,Rui Ding,Jinyu zhou,Zhonghao Yuan,Dan Li,Xuzhen Qin,Jiang Zhou,Zhili li
Background Altered glycosylation modulates the structure and function of disease-related proteins. The associations between serotransferrin (STF) N -glycosylation and liver diseases (LDs) have been revealed. However, how intact N -glycopeptides vary among different types of liver diseases remains unclear. Methods Intact STF N -glycopeptides from patients with chronic liver disease (CLD, n = 92), primary liver cancer (PLC, n = 123), metastatic liver cancer (MLC, n = 57), and healthy controls (HCs, n = 59) were determined using high-resolution mass spectrometry. Results Significant changes were displayed in STF glycosylation among 4 groups. The LD screening model, including Asn432 G1S/G2S, Asn432 G2S/G2S2, and Asn630 G2NS2/G2FNS2, was constructed to differentiate LDs from HCs, with a AUC of 0.92. The liver cancer (LC) diagnostic model, a combination of Asn432 G1-N/G1S-N, Asn432 G1/G2, Asn432 G2FS/G2FS2, and Asn630 G1S-N /G1S, showed good performance in discriminating LC from CLD (AUC = 0.93). Moreover, AFP-negative LC patients (93 %) were successfully predicted by the LC diagnostic model. Furthermore, the MLC triage model, composed of Asn432 G1/G2, Asn432 G3F/G3FS, Asn630 G2/G2S, Asn630 G2S2/G2NS2, and Asn630 G3FS/G3FS2, yielded an AUC of 0.98 between PLC and MLC. Conclusions STF N -glycosylation is a potential biomarker for the accurate classification of different LDs.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1855-1865
·
IF 5
Shuyi Yang,Jiayi Deng,Jiaying Chen,Qingmei Tan,Tianren Liu,Ke Chen,Dongxue Han,Yingming Ma,Mengjiao Dai,Li Niu
The conversion of N2 and CO2 into urea through a photocatalytic C–N coupling reaction under ambient conditions serves as a novel green avenue for urea synthesis. However, the poor adsorption and C–N coupling capability of inert gas molecules hinder the efficient catalytic activity. Herein, palladium-decorated CeO2 (Pd–CeO2) was demonstrated as an efficient photocatalyst for C–N coupling reaction and delivered a remarkable urea yield rate of 9.2 μmol h−1 g−1, which was superior to that of pristine CeO2 (2.5 μmol h−1 g−1). Comprehensive investigations further endorsed that the emerged space-charge region in the CeO2(111)/Pd(111) interface not only effectively facilitates the targeted capture and activation of inert CO2 and N2 but also stabilizes the formation of key intermediates (*NCON). Besides, the effective inhibition of the endothermic *NNH intermediate is conducive to the subsequent C–N coupling process and the improvement of reaction selectivity. The reaction mechanism was studied in detail by density functional theory (DFT) with the formation of a C–N bond via a thermodynamically spontaneous reaction between *NN* and CO. This work provides novel insights into the conversion of CO2 and N2 into urea.
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International Journal of Environmental Science and Technology
·
2023
·Vol. 20
·期 11
·11865-11876
·
IF 3.1
Xin X.,Liu H.,Sun J.,Gao K.,Jia R.
The composite material based on N- , S- , and Fe-doped TiO 2 (NSFe-TiO 2 ) synthesized by wet impregnation was used as a photocatalyst to rapidly degrade sulfadiazine. The photocatalytic degradation behavior and mechanism of sulfadiazine on NSFe-TiO 2 were investigated for revealing the role of degradation under ultraviolet light. The results showed that compared with TiO 2 , NSFe-TiO 2 markedly improved the efficiency in photocatalytic degradation of sulfadiazine: more than 90% of sulfadiazine could be removed within 120 min by NSFe-TiO 2 dosage of 20 mg L −1 . The process conformed to first-order reaction kinetics model. The parameters such as loaded amount of NSFe-TiO 2 , solution pH value, humic acid concentration and recycle numbers on removal efficiency were also studied. Compared to neutral and alkaline conditions, acidic condition was not conducive to the photocatalysis. HA, Ca 2+ , Cu 2+ and Zn 2+ in the actual water body had mild inhibition on sulfadiazine degradation in UV/NSFe-TiO 2 system. Fragments screened by high-resolution mass spectrometry were conducted to explore the oxidation mechanism and pathways of sulfadiazine degradation. On the whole, UV/NSFe-TiO 2 photocatalysis has a good effect on sulfadiazine removal.
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CONSTRUCTION AND BUILDING MATERIALS
·
2022
·
IF 7.693
Jieyu Sun,Xiuyi Lin,Yuhan Qiu,Runyu Wang,Yanfei Zhang,Chuanshuang Hu,Weiwei Zhang
Bamboo is an eco-friendly and sustainable material but with limited application due to its susceptibility to mold infection. N -methylol acrylamide (NMA) is a cross-linking monomer with bifunctional groups, here NMA was used to modified bamboo to enhance its anti-mold property through in situ polymerization and cross-linking reaction. When the monomer concentration was 6% and above, no mold germinated at the NMA treated bamboo surface. SEM/EDX, FTIR was used to explore the anti-mold mechanism of NMA modified bamboo. The primary reason for the improvement in the anti-mildew property was the coating effect of PNMA on starch as well as the antimicrobial properties of PNMA. Thermal stability of bamboo before and after modification was almost unchanged. Results also indicated that the mechanical properties of modified bamboo are improved by around 50%, which was mainly attributed to more compact structure of cell wall obtained in the neutral reaction condition. The NMA in situ polymerization was proved to be a potential modification for bamboo to broaden its application.
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 6
·981-987
·
IF 3.1
Nan Li,Minghao Shi,Wei Zhan,Wenjing Shen,Mianmian Wu,Guifang Sun,Qingfei Li,Jiangquan Ma
Ru-based catalysts are potential substitutes for Pt in the hydrogen evolution reaction (HER). It is worth noting that the Se ions in RuSe2 can modulate the electronic structure of the Ru metal, thus effectively improving the HER kinetics of RuSe2. However, single electronic structure modulation is hard to complete due to the electron deficiency of active Ru atoms. Herein, we prepare and design a novel RuSe2/Co–N–C (RuSe2 nanospheres supported on Co–N–C nanosheets) electrocatalyst with two-electron modulation by a hydrothermal and thermal annealing method. Benefiting from the uniform distribution of RuSe2 nanospheres on Co–N–C nanosheets and Co–N–C nanosheets acting as additional electron donors to make up for the electron deficiency of the Ru metal, RuSe2/Co–N–C exhibits excellent HER performance with a low overpotential of 26.4 mV at 10 mA cm−2 and a low Tafel slope of 53.2 mV dec−1. This work offers an effective method for the synthesis of high catalytic performance electrocatalysts by constructing an interaction between the carrier and the active metal.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2022
·
IF 5.895
Ruige Yang,Zhiyan Liu,Meiyue Han,Liping Cui,Yong Guo
To discover novel natural-product-based insecticide candidates, herein, a variety of osthole-derived N-benzoylthioureas were synthesized and assessed for their insecticidal activities against three insect pests. An insecticidal assay showed that most of the target osthole-derived N-benzoylthioureas displayed a more potent and broad-spectrum insecticidal effect than the parent osthole after the introduction of N-benzoylthioureas on the C-3′ position of osthole. Compound B24 displayed the most potent growth inhibitory (GI) effect on Mythimna separata Walker, with a final corrected mortality rate of 82.1% when treated with a concentration of 1 mg/mL, which was 1.64- and 1.53-fold higher in comparison to osthole and the botanical insecticide toosendanin, respectively. Compounds B22, B23, and B25 displayed a more promising aphicidal effect on Myzus persicae Sulzer, and their LD50 values were 0.015, 0.017, and 0.019 μg/larvae, respectively, superior to the commercially available insecticide rotenone (0.024 μg/larvae). Derivatives B19, B20, B23, and B25 displayed more potent larvicidal activity against Plutella xylostella Linnaeus, with LC50 values of 0.22, 0.26, 0.15, and 0.30 mg/mL, respectively, exceeding that of rotenone (0.37 mg/mL). Furthermore, both compounds B19 and B23 against P. xylostella were found to be more effective than rotenone in a control efficacy assay under greenhouse conditions. The structure–activity relationship (SAR) suggested that osthole-derived N-benzoylthioureas are more active in most cases when the R group is an electron-withdrawing group than when it is an electron-donating group, especially for halogenated groups. Additionally, the potent compounds B19 and B23 possessed good selectivity and were less toxic to non-target organisms. This study suggests that these osthole-derived N-benzoylthioureas could be further studied in depth as eco-friendly natural product pesticides in crop protection.
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