CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 6
·948-953
·
IF 3.1
Xu Henan,Zhang Lingling,Wang Huilin,Zhang Shaopeng,Li Wei,Wang Xiao,Song Shuyan,Wang Daguang,Shi Zhan
N anozymes have shown great potential for life sciences owing to their distinct advantages, such as low cost and high stability, compared with natural enzymes. Despite significant progress, state-of-art nanozymes commonly suffer from relatively low specific activities. Herein, we propose a promising to address this issue by creating single-atom nanozymes. A ball-milling-assisted strategy has been developed to induce the transformation of Cu species from bulk to single atoms. The highly-simplified steps allow a large-scale synthesis, that over 4.2 g of single-atom Cu−N doped carbon nanozymes can be achieved in one pot. It exhibits a remarkably improved peroxidase-like activity and stability compared with N doped C anchored Cu nanoparticles. Further experimental firmly reveals the crucial role of the single-atom Cu site that can generate more active ·OH species for boosting the catalytic process.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Zhang Jin,Guo Chenxi,Fang Susu,Zhao Xiaotong,Li Le,Jiang Haoyang,Liu Zhaoyang,Fan Ziqi,Xu Weigao,Xiao Jianping,Zhong Miao
Electrochemical CO 2 reduction (CO 2 R) to ethylene and ethanol enables the long-term storage of renewable electricity in valuable multi-carbon (C 2+ ) chemicals. However, carbon–carbon (C–C) coupling, the rate-determining step in CO 2 R to C 2+ conversion, has low efficiency and poor stability, especially in acid conditions. Here we find that, through alloying strategies, neighbouring binary sites enable asymmetric CO binding energies to promote CO 2 -to-C 2+ electroreduction beyond the scaling-relation-determined activity limits on single-metal surfaces. We fabricate experimentally a series of Zn incorporated Cu catalysts that show increased asymmetric CO* binding and surface CO* coverage for fast C–C coupling and the consequent hydrogenation under electrochemical reduction conditions. Further optimization of the reaction environment at nanointerfaces suppresses hydrogen evolution and improves CO 2 utilization under acidic conditions. We achieve, as a result, a high 31 ± 2% single-pass CO 2 -to-C 2+ yield in a mild-acid pH 4 electrolyte with >80% single-pass CO 2 utilization efficiency. In a single CO 2 R flow cell electrolyzer, we realize a combined performance of 91 ± 2% C 2+ Faradaic efficiency with notable 73 ± 2% ethylene Faradaic efficiency, 31 ± 2% full-cell C 2+ energy efficiency, and 24 ± 1% single-pass CO 2 conversion at a commercially relevant current density of 150 mA cm −2 over 150 h.
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PubMed
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2023
·
IF 6.8
Jie Luo,Mingzhi Zhang,Yang Deng,Haohuan Li,Qinglong Bu,Rui Liu,Jiansheng Yu,Shanshan Liu,Ze Zeng,Wei Sun,Ganbei Gui,Xicheng Qian,Yinglun Li
Studies on the general toxicity of copper nanoparticles (Cu NPs) have been conducted extensively, but their effects on reproductive toxicity remain unclear. In this study, we evaluated the toxic effect of Cu NPs on pregnant rats and their litter. The comparative in vivo toxicity of Cu ions, Cu NPs, and Cu microparticles (MPs) was studied in a 17-day repeated oral-dose experiment at the doses of 60, 120, and 180 mg/kg/day in pregnant rats. The pregnancy rate, mean live litter size, and number of dams decreased when exposed to Cu NPs. Moreover, Cu NPs caused a dose-dependent increase in ovarian Cu levels. The metabolomics results showed that Cu NPs caused reproductive dysfunction by altering sex hormones. In addition, in vivo and in vitro experiments showed that the ovarian cytochrome P450 enzymes (CYP450), responsible for hormone production, were significantly upregulated, whereas the enzymes responsible for hormone metabolism were significantly inhibited, resulting in a metabolic imbalance in some ovarian hormones. Furthermore, the results revealed that the nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB) and mitogen-activated protein kinase (MAPK) signaling pathways significantly participated in the regulation of ovarian CYP enzyme expression. Overall, the results of the in vivo and in vitro toxicity experiments with Cu ions, Cu NPs, and Cu MPs suggested that toxicity from nanoscale Cu particles poses a more serious reproductive threat than microscale Cu as Cu NPs could directly damage the ovary and affect the metabolism of ovarian hormones.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Zeqing Hu,Rong Wei,Chen Yan,Han Wan,Yu Liu,Longjiu Cheng,Zhou Li,Jiming Song
In this work, carrier concentration optimization and effective mass increase of Cu2GeSe3, which were considered to be a synergetic effect of electrical transport properties, were achieved by the co-doping of Bi and Zn on the Cu site. This effect led to a higher Seebeck coefficient of ∼307.76 μV K–1 at 723 K for the Cu1.988Bi0.01Zn0.002GeSe3 sample. This effect also resulted in a higher power factor of ∼8.66 μW cm–1 K–2 at 723 K and an average power factor of ∼6.29 μW cm–1 K–2 at the temperature range of 303–723 K for the Cu1.988Bi0.01Zn0.002GeSe3 sample, which were ∼135 and ∼196% larger than those of pristine Cu2GeSe3, respectively, and are among the highest value of the Cu2GeSe3-based sample. Benefiting from simultaneous optimization of the power factor, the maximum ZT of ∼0.75 for the Cu1.988Bi0.01Zn0.002GeSe3 sample at 723 K was obtained, which is ∼288% higher than that of Cu2GeSe3.
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Carbon Energy
·
2023
·Vol. 5
·期 11
·e343
·
IF 20.5
Xin Liu,Kun Wang,Ying Liu,Fuhua Zhao,Jianjiang He,Hao Wu,Jianfei Wu,Han-Pu Liang,Changshui Huang
The inherent shortcomings of a zinc anode in aqueous zinc-ion batteries (ZIBs) such as zinc dendrites and side reactions severely limit their practical application. Herein, to address these issues, an ion-oriented transport channel constructed by graphdiyne (GDY) nanowalls is designed and grown in situ on the surface of a zinc electrode. The vertically stacked GDY nanowalls with a unique hierarchical porous structure and mechanical properties form a nanomesh-like interface on the zinc electrode, acting as an ion-oriented channel, which can efficiently confine the segmented growth of zinc metal in microscopic regions of hundreds of nanometers. In those microscopic regions, the uniform domain current density is effortlessly maintained compared with a large surface area, thereby inhibiting zinc dendrites effectively. Besides, due to the presence of the ion-oriented channel, the modified zinc anode demonstrates long-term stable zinc plating/stripping performance for more than 600 h at 1 mAh cm −2 in an aqueous electrolyte. In addition, full-cells coupled with MnO 2 show high specific capacity and power density, as well as excellent cycling stability with a capacity retention of 82% after 5000 cycles at 1 A g −1 . This work provides a feasible and accessible surface engineering approach to modify the electrode interface for confined and dendrite-free zinc deposition in aqueous ZIBs.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2023
·
IF 5.7
Liangliang Tang,Dongxu Yao,Yongfeng Xia,Hanqin Liang,Yu-Ping Zeng
Gas-pressure sintered silicon nitride (Si 3 N 4 ) ceramic was brazed to oxygen-free copper (OFC) foil using 20.22 ± 0.93 mg/cm 2 of Ag-Cu-TiH 2 filler at 875 ◦ C for 0.5 h. The effect of TiH 2 content on the 3D morphology, including the cross-section microstructure and etched surface morphology of Si 3 N 4 ceramic/OFC foil joints, was analyzed. An evolution model of the interfacial microstructure for joints was proposed based on 3D morphological analysis. The reaction between the brazing alloy and Si 3 N 4 ceramic formed the interfacial reaction layer and the inside reaction zones during brazing. The growth mechanism of the interfacial reaction layer was discussed in detail. The peeling test was used to evaluate the bonding strength of the Si 3 N 4 ceramic/OFC foil joints, and the optimum peeling strength of 25.1 N/mm was achieved at 5 wt% TiH 2 content. The interfacial microstructure of the joints changed with TiH 2 content, leading to different main fracture mechanisms and corresponding peeling strengths.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 13
·5587-5598
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IF 4.5
Sun Shanshan,Zhang Zihao,Li Shuhan,Le Jinxun,Qian Haixia,Yin Xiaoshuang,Liu Ying,Yang Wenzhong,Chen Yun
Magnetic core–shell nanomaterial Fe 3 O 4 –SiO 2 –Cu 2 O/Cu was first successfully synthesized using an economical strategy. Using Fe 3 O 4 as a magnetic center for easy recycling and SiO 2 as the connecting layer, Cu elements were evenly and steadily distributed on the surface of the Fe 3 O 4 –SiO 2 –Cu 2 O/Cu core–shell nanostructure. The magnetic catalyst performed outstanding catalytic reduction activity for 4-nitrophenol (4-NP), and the complete catalytic reduction of 4-NP was achieved within only 5 min. What’s more, the catalyst could be well recycled, and the catalytic efficiency remained more than 90% after being reused 24 times. Graphical abstract
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Joule
·
2023
·
IF 39.8
Tiancheng He,Haiyan Wang,Bing Lu,Tianlei Guang,Ce Yang,Yaxin Huang,Huhu Cheng,Liangti Qu
Ubiquitous moisture is of particular attraction for sustainable power generation. However, rigorous assembly procedures limit the efficient large-scale integration for moisture-enabled electric generators (MEGs). Herein, we develop fully printed planar MEG (PMEG) arrays using modulated polycation and polyanion inks, which maximize access to moisture and make it free of strict assembly and device packaging. Thus, a PMEG unit (only 0.3 cm 2 ) generates an open-circuit voltage of up to 1.1 V, along with a power density of 2.6 μW cm −2 . A small piece of sheet with 200 PMEG units offers a maximum voltage of 200 V and a current of 1.3 mA. A standard power module is constructed to meet the on-demand power supply requirements of compact electronics. Furthermore, scalable and customizable PMEG arrays can be compatibly integrated with flexible circuits, as demonstrated by a fully printed self-powered functional system including PMEG arrays and energy-storage and electrochromic devices.
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Xupeng Zhu,Jun Zhang,Jun Liao,Qiang Ru,Wenfeng Fu,Zhiguo Wang,Shuwen Xue
Return to the physics origin of Cu 2 ZnSnS 4 type (CZTS-type, include CZGS, CZGTS, CZTSSe, etc.) material system, studying the influence of replacement elements on the optoelectronic properties by preparing high-quality single crystal materials to clarify the relationship between the key defect states of materials and carrier dynamics is the only way which must be passed to find efficient paths to improve the existing performance of CZTS-type optoelectronic devices. Herein, the optical behavior of high-quality Cu 2 ZnGe x Sn 1-x S 4 (CZGTS) single crystal prepared by the molten salt method and its relationship with Ge content were systematically studied using a photoluminescence (PL) and absorption tests at room temperature. Combined with the simple electrical tests, the transformation of carrier recombination mechanism as increasing the Germanium content in CZGTS single crystal before and after phase transition were reported for the first time. The transmission electron microscopy images, X-ray diffraction spectra and Raman scattering spectra of CZGTS were adopted to reveal the evolution mechanism of single crystal growth and phase transition caused by the change of Ge composition. The results show that the tunable blue-shift of PL peak emerges with the increase of Ge content and the excitation power dependence has a saturation phenomenon in the CZGTS single crystal particles. In consideration of the optical bandgap, PL peak position, PL intensity, carrier lifetime and the macroscopic resistivity, it is confirmed that the intrinsic PL behavior could be effectively tailored by different Ge amounts. Compared with the recombination PL of interband carrier (E p > E g ) in Cu 2 ZnSnS 4 , the band tailed carriers (E p < E g ) dominated by defect states would play a powerful role in CZGTS single crystal. Our work provides a strategy for tailoring the bandgap of CZGTS materials and a new perspective for understanding the influence of defect states on carrier dynamics.
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Nano Research
·
2023
·Vol. 16
·期 6
·8497-8503
·
IF 9.9
Zou Jian,Wu Zhenrui,Tang Ruilin,Ren Zhenzhen,Niu Xiaobin,Wang Liping
Copper sulfide (CuS) is a promising cathode for lithium-ion batteries (LIBs) due to its impeccable theoretical energy density (∼ 1015 Wh·kg −1 and 4743 Wh·L −1 ). However, it suffers from voltage decay leaded energy density loss and low energy efficiency, which hinders its application. In this work, with combined ex-situlin-situ X-ray diffraction (XRD) and electrochemical analysis, we explore detailed degradation mechanisms. For the voltage decay, it is attributed to a spontaneous reaction between CuS cathode and copper current collector (Cu CC). This reaction leads to energy density loss and active materials degradation (CuS → Cu 1.81 S). As for energy efficiency, CuS undergoes a series of phase transformations. The main phase transition processes are CuS → α -LiCuS → Li 2− x Cu x S + Cu → Li 2 S + Cu for discharge; Li 2 S + Cu → Li 2− x Cu x S → β -LiCuS → CuS for charge. Here, α -LiCuS, β -LiCuS, and Li 2− x Cu x S are newly identified phases. These phase changes are driven by topotactic-reaction-related copper diffusion and rearrangement. This work demonstrates the significance of transition-metal diffusion in the intermediates formation and phase change in conversion-type materials.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Peng Xu,Pengfei Zhu,Xin Liu,Zhuoyu Yang,Jingwei Ma,Qiulai He
Fe 2+ activated peroxodisulfate (Fe 2+ /PDS) system has been widely studied for its efficient degradation of pollutants. However, the slow circulation of Fe 3+ /Fe 2+ greatly restricted the application of the system. In the study, AOII was significantly degraded by using Fe 3+ coupled with Cu 0 activate PDS system (Fe 3+ /Cu 0 /PDS system). Compared with the traditional Fe 2+ /PDS system, the Fe 3+ /Cu 0 /PDS system greatly improved the degradation of AOII and the decolorization rate reached 80.6 % within 30 min. The quenching experiments and electron spin resonance (EPR) showed that both hydroxyl radical (•OH) and sulfate radical (SO 4 •− ) were the mainly primary reactive oxygen species in the Fe 3+ /Cu 0 /PDS system with the contribution rates of SO 4 •− and •OH being 60.54 % and 25.06 % respectively. In the Fe 3+ /Cu 0 /PDS system, Cu 0 formed Cu + through H + corrosion and PDS/O 2 oxidation . Then, Cu + oxidized by O 2 to produce H 2 O 2 and Fe 3+ was reduced by Cu 0 and Cu + to form Fe 2+ . Finally, Cu + and Fe 2+ catalyzed PDS to generate SO 4 •− , and •OH was yield by the process of Cu + and Fe 2+ induced H 2 O 2 and the reaction of OH − /H 2 O and SO 4 •− . Common water matrices such as NO 3 − and SO 4 2− had no effect on the degradation, while Cl − promoted the degradation, and CO 3 2− and fulvic acid inhibited the degradation of AOII. Over 68.5 % of AOII was degraded in the experimental water samples and the Fe 3+ /Cu 0 /PDS system had great degradation performances in practical water sample of other contaminants. Moreover, the final discharge of total dissolved copper was <1 mg/L after sediment and filtering.
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Acta Metallurgica Sinica-English Letters
·
2023
·Vol. 36
·期 6
·1023-1037
·
IF 3.5
Fan Wenhao,Zhao Jianxun,Liu Dayong,Liang Qingcheng,Liu Wanqiang,Wang Qingshuang,Liu Heng,Chen Peng,Gao Shang,Bao Xinlong,Cheng Yong,Wang Xinwei,Guo Xin
Co 0.9 Cu 0.1 Si alloy was prepared by mechanical alloying method. Nitrogen-doped graphene (NG) and nitrogen–sulfur co-doped graphene (NSG) were prepared by hydrothermal method. 5 wt% graphene oxide, NG and NSG were doped into Co 0.9 Cu 0.1 Si alloy, respectively, by ball milling to improve the electrochemical hydrogen storage performance of the composite material. X-ray diffraction and scanning electron microscopy were used to characterize the structure and morphology of the composite material, and the LAND battery test system and three-electrode battery system were used to test the electrochemical performance of the composite material. The composite material showed better discharge capacity and better cycle stability than the pristine alloy. In addition, in order to study the optimal ratio of NSG, 3%, 5%, 7% and 10% of NSG were doped into Co 0.9 Cu 0.1 Si alloy, respectively. Co 0.9 Cu 0.1 Si alloy doped with 5% NSG had the best performance among all the samples. The best discharge capacity was 580.1 mAh/g, and its highest capacity retention rate was 64.1%. The improvement in electrochemical hydrogen storage performance can be attributed to two aspects. On the one hand, the electrocatalytic performance of graphene is improved by co-doping nitrogen and sulfur, on the other hand, graphene has excellent electrical conductivity.
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