MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Xijun Li,Sifan Zhang,Lihua Zhu,Jun Liu,Huan Zhang,Ning Zhao,Bing Hui Chen
Herein, a series of the Pt-based bimetallic catalysts (PtM x /SBA-15) are gained by using ultrasonic incipient wetness impregnation method (M = Co, Cu, Ni or Zn). The experimental results show that the catalytic performance (including catalytic activity (turnover frequency-TOF), selectivity to crotyl alcohol) of PtCo x /SBA-15 for catalyzing crotonaldehyde selective hydrogenation is the best among PtM x /SBA-15. Additionally, the ratio of Pt/Co in the PtCo x /SBA-15 catalysts is changed to successfully synthesize PtCo/SBA-15, PtCo 2 /SBA-15, PtCo 5 /SBA-15. It demonstrates that the selectivity of the PtCo x /SBA-15 catalysts for crotonaldehyde selective hydrogenation to crotyl alcohol is significantly improved with the increase of the Co content. The PtCo 5 /SBA-15 catalyst provides 83.8% conversion of crotonaldehyde, 94.3% selectivity to crotyl alcohol and TOF of 910.5 h −1 under mild reaction conditions (3.0 MPa H 2 , 80 °C and 2.0 h). And PtCo 5 /SBA-15 has much better catalytic performance (higher catalytic activity and selectivity to crotyl alcohol) than PtCu 5 /SBA-15, PtNi 5 /SBA-15 and PtZn 5 /SBA-15. The reasons are as follows: (1) PtCo alloy forms, which is conducive to crotonaldehyde adsorption and activation; (2) there is an appropriate synergy effect between Pt and Co, greatly improving the capacity of the catalyst activating hydrogen under mild conditions; (3) the electron transfers from Co to Pt, resulting in the increase of Pt electron density and decrease of Co electron density, then the Co sites are advantageous to C O group adsorption and activation and Pt sites for H 2 adsorbing and activating; (4) with the increase of the Co proportion in PtCo x /SBA-15, the synergy effect between Pt and Co in PtCo alloy strengthens and thus increases the selectivity of C O group hydrogenation.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 16
·2214215
·
IF 19
Xiaosong Hu,Xinyu Liu,Xin Hu,Chaoyue Zhao,Qingxin Guan,Wei Li
Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N 4 sites and low valence CuN x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N 4 and N 4 structures, which show strong Lewis basicity and has strong adsorption for *CO 2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO 2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO 2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO 2 . In the catalytic process, CuN x not only adsorbs and activates H 2 , but also cooperates with the adjacent Zn-N 4 and N 4 structures to jointly activate CO 2 molecules and further promotes the hydrogenation of CO 2 . This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
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International Journal of Bioprinting
·
2023
·
IF 8.4
Zhijing He,Chen Jiao,Junnan Wu,Jiasen Gu,Huixin Liang,Lida Shen,Youwen Yang,Zongjun Tian,Changjiang Wang,Qing Jiang
Porous hydroxyapatite (HA) scaffolds prepared by three-dimensional (3D) printing have wide application prospects owing to personalized structural design and excellent biocompatibility. However, the lack of antimicrobial properties limits its widespread use. In this study, a porous ceramic scaffold was fabricated by digital light processing (DLP) method. The multilayer chitosan/alginate composite coatings prepared by layer-by-layer method were applied to scaffolds and Zn 2+ was doped into coatings in the form of ion crosslinking. The chemical composition and morphology of coatings were characterized by scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). Energy dispersive spectroscopy (EDS) analysis demonstrated that Zn 2+ was uniformly distributed in the coating. Besides, the compressive strength of coated scaffolds (11.52 ± 0.3 MPa) was slightly improved compared with that of bare scaffolds (10.42 ± 0.56 MPa). The result of soaking experiment indicated that coated scaffolds exhibited delayed degradation. In vitr o experiments demonstrated that within the limits of concentration, a higher Zn content in the coating has a stronger capacity to promote cell adhesion, proliferation and differentiation. Although excessive release of Zn 2+ led to cytotoxicity, it presented a stronger antibacterial effect against Escherichia coli (99.4%) and Staphylococcus aureus (93%).
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PubMed
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 46
·e202202684
·
IF 2.307
Dehui Kong,Wenyu Xie,Jinxiong Wu,Xiuling Yan,Andrei Ivanets,Lijuan Zhang,Shasha Chu,Bo Yang,Bekchanov Davronbek,Xintai Su
Graphical Here, we used a two-phase solvothermal method to prepare electroplating sludge into LDHs. the conditions for the formation of LDHs were achieved by sodium oleate intercalation and the addition of divalent metal ions to prepare a material with a layered nanostructure. The adsorption of Congo red was mainly realized by surface metal complexation, formation of hydrogen bond and electrostatic attraction. It is a challenge to achieve the harmless treatment and resourceful use of various metal elements in electroplating sludge, and converting them into functional materials has become an important technological direction. Based on the existence of various metal ions in electroplating sludge, sodium oleate intercalated Zn−Cr-LDHs (Zn−Cr-layered double hydroxides) were prepared by two-phase solution heating method. The adsorption process of the prepared LDHs for Congo red (CR) in aqueous solution can be described by Langmuir isotherm model and pseudo-second-order kinetic model and the maximum adsorption capacity is 2750.43 mg/g. The results of TEM and XPS show that the adsorption mechanism is dominated by electrostatic adsorption, ion exchange process, hydrogen bonding interaction and surface complexation. Therefore, this paper provides a strategy for recovering metal elements from electroplating sludge to prepare LDHs adsorption materials with ultra-high adsorption capacity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Lian Xue,Ying Shi,Cunping Huang,Qiang Wu,Bingbing Chen,Weifeng Yao
Effective and affordable photocatalysts play an important role in the cost reduction of solar hydrogen production through photocatalytic water splitting. In this research, a Zn 2+ and Ni 2+ modified carbon hydrogen evolution cocatalyst (ZnNi-C) were synthesized and immobilized onto the surface of CdS (CdS@ZnNi-C) for photocatalytic hydrogen evolution (PHE). The preparation used an ethylenediaminetetraacetic acid disodium (EDTA)-assisted method. The hydrogen evolution rate and apparent quantum efficiency (AQE) at 420 nm for an optimized CdS@ZnNi-C photocatalyst are15.7 mmol/h/g and 31.4 %, respectively. The rate is 2.4 times and 3.7 times greater than those of Zn 2+ and Ni 2+ modified carbon cocatalysts (Zn-C) and (Ni-C) on CdS (CdS@Zn-C) and (CdS@Ni-C), respectively. Density functional theory calculations indicate that the elevated catalytic performance of CdS@ZnNi-C is due to the co-anchored Zn 2+ and Ni 2+ in carbon layers that lead to a favorable Gibbs free energy (ΔG H *) for hydrogen evolution. This approach is valuable for the design of stable and efficient photocatalysts for renewable hydrogen production.
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ACS Nano
·
2022
·
IF 18.027
Yang-feng Cui,Zhen-bang Zhuang,Zi-long Xie,Ren-fei Cao,Qi Hao,Ning Zhang,Wan-qiang Liu,Yun-hai Zhu,Gang Huang
Alkaline Zn–MnO2 batteries feature high security, low cost, and environmental friendliness while suffering from severe electrochemical irreversibility for both the Zn anode and MnO2 cathode. Although neutral electrolytes are supposed to improve the reversibility of the Zn anode, the MnO2 cathode indeed experiences a capacity degradation caused by the Jahn–Teller effect of the Mn3+ ion, thus shortening the lifespan of the neutral Zn–MnO2 batteries. Theoretically, the MnO2 cathode undergoes a highly reversible two-electron redox reaction of the MnO2/Mn2+ couple in strongly acidic electrolytes. However, acidic electrolytes would inevitably accelerate the corrosion of the Zn anode, making long-lived acidic Zn–MnO2 batteries impossible. Herein, to overcome the challenges faced by Zn–MnO2 batteries, we propose a hybrid Zn–MnO2 battery (HZMB) by coupling the neutral Zn anode with the acidic MnO2 cathode, wherein the neutral anode and acidic cathode are separated by a proton-shuttle-shielding and hydrophobic-ion-conducting membrane. Benefiting from the optimized reaction conditions for both the MnO2 cathode and Zn anode as well as the well-designed membrane, the HZMB exhibits a high working voltage of 2.05 V and a long lifespan of 2275 h (2000 cycles), breaking through the limitations of Zn–MnO2 batteries in terms of voltage and cycle life.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 11
·110538
·
IF 4.386
Can Fang,Qingfeng Yi,Aling Chen,Yuebing Wang,Yaping Wang,Xiaofang Li
Zn-air battery, like other electrochemical power devices such as fuel cells, has the advantages of environmental friendliness and high energy convert efficiency. One of the main problems facing Zn-air battery is how to improve the electrocatalytic activity of the cathode catalyst with low cost and simple preparation process. Herein, N-doped carbon nanosheets/nanotubes composite loaded Fe-Co nanoparticles were prepared via a facile pyrolysis of the solid mixture composed of dicyandiamide, sucrose, cobalt nitrate, iron nitrate, iron phthalocyanine (FePc) and cobalt phthalocyanine (CoPc). The samples were well characterized and their electroactivity towards oxygen reduction reaction (ORR) was tested in a full pH range including acidic, neutral and alkaline media. In 0.1 mol l−1 KOH solution, the ORR onset potential and half-wave potential of the FeCo-FePc/NTu-CNsh are 1.03 V and 0.91 V, which are very close to the performance of commercial Pt/C catalyst (40%). In neutral solution (1 M KCl+4 M NH4Cl), FeCo-FePc/NTu-CNsh presents an ORR onset potential of 0.93 V and half-wave potential of 0.82 V, which are superior to Pt/C with onset potential of 0.92 V and half-wave potential of 0.81 V. The home-made Zn-air battery with the prepared samples as the cathodic catalysts reveal excellent performance, and the FeCo-FePc/NTu-CNsh Zn-air battery presents a maximum power density of 281.8 mW·cm−2 as well as the high stability at different discharging current densities.
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Nanoscale
·
2022
·Vol. 14
·期 24
·8640-8648
·
IF 8.307
Tao Chen,Changyu Yang,Xuewen Hu,Qicheng Zhang,An Cai,Huibin Liu,Yang Li,Wenchao Peng,Fengbao Zhang,Xiaobin Fan
Aqueous rechargeable zinc-ion batteries (ZIBs) are emerging in grid energy storage due to zinc abundance and intrinsic safety. However, developing suitable cathode materials with satisfactory stability and rate capacity remains a great challenge. Herein, a structure of layered MXene derived nanoporous VOx wrapped with graphene nanosheets (rGO–VOx) is constructed as a cathode for ZIBs. The incorporation of two typical 2D materials imparts composites with shortened diffusion pathways and increased electrical conductivity. Thus, the rGO–VOx cathode exhibits a remarkable rate capability of 196 mA h g−1 at 8 A g−1 and long-term stability with 90% retention after over 1200 cycles at 5 A g−1 in an aqueous coin cell. The Zn storage mechanism is also systematically investigated. The layered V2O5 transforms into layered ZnxV2O5·nH2O with larger interspacing upon cycling. NaV6O15 and the in situ formed ZnxV2O5·nH2O co-contribute to the subsequent insertion and extraction process.
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高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Jiali Song,Yu Gao,Guoguo Tan,Qikui Man,Zhi Wang
Spinel ferrites are widely used for electromagnetic wave (EMW) absorption applications. In this study, spinel Ni–Zn ferrites with excellent microwave absorption properties were synthesized. Their EMW absorption characteristics and interaction mechanisms were studied to lay the foundation for the study of the role of Ni–Zn ferrite as a magnetic substrate for composites. Herein, Ni 0 · 5 Zn 0 · 5 Fe 2 O 4 was prepared by the hydrothermal method (H-NZFO) and the sol–gel auto-combustion method (S-NZFO); both samples exhibited distinct microwave absorption properties. The S-NZFO absorber (thickness = 3.72 mm) demonstrated the best dual-zone microwave absorption with two strong reflection loss peaks at 5.1 and 10.5 GHz. The corresponding effective absorption bandwidth (EAB) reached 9.0 GHz, which covered part of the S-band and all of the C- and X-bands. These results were attributed to the high saturation magnetization, outstanding complex permeability, and multiple magnetic loss channels of S-NZFO. The H-NZFO sample exhibited excellent absorption capability and matching thickness. At a thickness as low as 1.71 mm, the minimum reflection loss ( RL min ) of the H-NZFO absorber reached -60.2 dB at 13.1 GHz. The maximum bandwidth corresponding to RL below -10 dB was 4.6 GHz. These results can be attributed to small particle size, high complex permittivity, and multiple dielectric loss channels of H-NZFO. The observed wide effective absorption bandwidth of S-NZFO and strong microwave absorption capability of H-NZFO suggest the potential of both materials as substrates for efficient microwave absorbers in military as well as civilian absorption applications.
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Virtual and Physical Prototyping
·
2022
·
IF 10.962
Mingli Yang,Yang Shuai,Youwen Yang,Da Zeng,Shuping Peng,Zongjun Tian,Cijun Shuai
Carbon nanofibre (CNF) is a potential reinforcement in Zn implants. Nevertheless, its poor interfacial compatibility reduces the reinforcement efficiency drastically. In this study, rare earth lanthanum (La) was used as a compatible interface layer between CNF and Zn matrix. On the one hand, La in situ grew on acidified CNF by a chemical synthesis and achieved a firm coordination covalent bond with the oxygenated functional group derived from CNF. On the other hand, La, as an active rare earth element, could carry out the alloying reaction with the Zn matrix, thus forming strong metal bonding. Results showed that the tensile strength of composites was enhanced from 180.2 ± 12.1 to 243.4 ± 10.2 MPa since the La interface layer promoted the transfer of the interfacial shear stress from the Zn matrix to CNF and thereby consumed massive fracture energy. Encouragingly, it simultaneously improved the ductility, as La activated basal slip and improved the dislocation accommodation capacity. Moreover, the Zn implants displayed excellent anti-tumour efficiency.
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FUEL
·
2022
·
IF 8.035
Zixuan Ma,Fenghai Cao,Yuhao Yang,Liyan Wang,Tao Zhang,Minghui Tan,Guohui Yang,Yisheng Tan
Bifunctional catalysts composed of ZnCrO x oxide and ZSM-5 were widely used in syngas-to-aromatics (STA). The CO conversion on bifunctional catalysts was generally higher than that on oxide catalysts attributed to the pulling effect of zeolite, but the key factor for the improvement of CO conversion was still short of systematical explanation. In this work, the degree of nonstoichiometric spinel of ZnCrO x (ZxC) oxides was finely tuned through modulating the ratio of Zn/Cr, which could significantly influence the catalytic behaviors of ZnCrO x /ZSM-5 catalysts for the CO hydrogenation to aromatics. The increase of nonstoichiometric spinel corresponded to the increase of oxygen vacancies and the enhancement of Zn-Cr synergistic effect, which promoted the activation of H 2 and CO, leading to a dramatic increase of CO conversion. The work revealed that the action of ZnO and oxygen vacancies was the key factor for CO pulling in ZnCrO x oxide and ZSM-5 catalyzed STA reaction.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Qichen,Feng Qingguo,Lei Yongpeng,Tang Shuaihao,Xu Liang,Xiong Yu,Fang Guozhao,Wang Yuchao,Yang Peiyao,Liu Jingjing,Liu Wei,Xiong Xiang
Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm −2 ), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate and robust quasi-solid-state Zn-air battery enabled by atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode and a polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified by the addition of dimethyl sulfoxide. This design enables a cycling current density of 100 mA cm −2 over 50 h at 25 °C. A low-temperature cycling stability of over 300 h (at 0.5 mA cm −2 ) with over 90% capacity retention at −60 °C and a broad temperature adaptability (−60 to 60 °C) are also demonstrated.
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