CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Qiwen Pan,Fei Lin,Ruiqi Liu,Yilin Li,Xinyue Zhang,Rui Luo,Lingling Cai,Yang Liu,Wuguo Deng,Liru He
Nanocatalysts provide a platform for developing anti-tumor strategies by activating intratumoral chemical catalysis to produce highly toxic reactive oxygen species (ROS). However, the biological effect of nanocatalysts on tumor cells, which is pivotal for effective nanotherapy treatment, remains poorly understood. Herein, we present a general and facile method of synthesizing Fe/Ni-layered double hydroxides (LDHs) for enhanced apoptosis- and ferroptosis-induced cancer nano-therapy, as well as a potential mechanism underlying the anti-tumor effect based on transcriptome sequencing. An analysis of the chemical structure suggests that the Fe atoms interact strongly with the Ni atoms in Fe/Ni-LDH. Compared with Fe-OH and Ni-OH, Fe/Ni-LDH exhibited significantly better ROS-catalytic activity, with a V max of 5.015 × 10 −2 μM·s −1 , and generated massive amounts of •OH and O 2 •− radicals, enabling outstanding chemo-dynamic therapy. Both in vitro and in vivo experiments indicated a robust apoptosis-induced cell death pathway, increased intracellular oxidative stress, and accumulation of lipid peroxide (LPO), promoting ferroptosis-involved cancer-cell death, which was further confirmed by transcriptome sequencing. The Fe/Ni-LDH biocatalyst not only provides a robust nanoplatform for tumor suppression but also encourages further exploration and applications of nanobiocatalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
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IF 8.4
Yiyu Chen,Huiting Lian,Bin Liu,Guangming Liu,Xiaofeng Wei
Food allergy diagnosis requires a highly sensitive detection of allergen-specific immunoglobulin E (sIgE) in the serum. Enzyme-linked immunosorbent assay (ELISA) is a classical method widely used for sIgE detection but had to rely on costly and time-consuming assay procedures, skilled technicians, and bulky equipment. Here, a multiplexed origami paper analytical device (moPAD) that is hexahistidine-tagged and integrated with a nitrilotriacetic acid-functionalized surface with nickel (Ni-NTA) was developed to achieve low-cost and high-efficiency immunosensing of multiple allergen-specific IgEs in serum. The major oyster allergens, Cra a 1, Cra a 2, and Cra a 4, were used to detect sIgE in human serum. The feasibility of the moPAD-based immunosensing strategy was successfully demonstrated by desirable sensitivities for multiple targets. The detection results of moPAD for 72 serum samples were 100% consistent with clinical test results, while 69 of these results showed no significant differences from ELISA results, demonstrating the accuracy and stability of this method. A fully integrated moPAD reduces detection time and achieves highly sensitive quantification using a simple smartphone-based readout. Efficient allergen modification of paper devices has great applicability in allergen component-resolved diagnostics. The implementation of moPAD can make the process of allergy diagnosis simpler for patients, physicians, and healthcare systems alike.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Jingjing Niu,Zhe Xue,Jiuchao Tang,Saravanan Rajendran,Xinyu Zhang,Jiaqian Qin
Developing efficient, economic, and environment-friendly electrocatalysts to meet the industrialized hydrogen evolution reaction (HER) needs is highly desired for dealing with the energy crisis. Under the known premise, how to reasonably control the doping amount of copper greatly influences the structure and is one of the key factors affecting the performance of the catalyst. Herein, a series of Ni–Cu–C electrocatalysts are successfully synthesized through a simple electrodeposition method. The unique dendritic morphology can be obtained by adjusting the different glucose concentrations . DFT simulation reveals that the proper proportion of copper can significantly modulate the H adsorption-free energy Δ G H ∗ It can boost the intrinsic activity of Ni–Cu–C catalysts. NCC-3 delivers an overpotential of 87 mV and 165 mV in alkaline media at the current density of 10 mA cm −2 and 100 mA cm −2 , respectively and presents outstanding long-term stability for 50 h. Such excellent HER activity stems from a large ECSA area and better electron-transfer ability. The study presents a feasible way to control metal alloy catalysts' composition in the electrodeposition process .
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Hong Du,Xiuyun Ma,Miao Jiang,Siyuan Zhao,Qi Fang,Xiumei Liu,Zongchao Conrad Zhang
Xylitol is a value-added health product from the hemicellulose component in biomass. In this work, highly efficient Cu–Ni/SiO2 catalysts are developed for the production of xylitol by means of xylose hydrogenation. The bimetallic catalysts exhibit higher activity compared to the corresponding monometallic nickel or copper catalyst and the currently used industrial Raney nickel catalyst. The bimetallic catalyst with a higher ratio of nickel to copper shows a better performance. The 5Cu15Ni/SiO2 catalyst exhibits a xylose conversion of 96% accompanied by higher than 99% selectivity to xylitol under the moderate conditions of 100 °C and 3MPa H2. The bimetallic catalysts show improved performances when they are activated at a low temperature. The apparent activation energies of xylose hydrogenation over the 5Cu15Ni/SiO2 and 20Ni/SiO2 catalysts are 16.6 and 25.2 kJ/mol, respectively. The formation of the Cu–Ni alloy leads to a lower activation energy and thus superior performance for xylose hydrogenation to xylitol.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Wei Peng,Zhaoyang Wang,Ruihu Lu,Qi Li,Ziyun Wang,Yan Zhao,Lin Xu,Liqiang Mai
Developing highly-active and robust electrocatalysts for the hydrogen evolution reaction (HER) is extremely desirable for hydrogen production but remains highly challenging. Herein, we reported a rational strategy to fabricate a novel metallic heterostructure composed of defect-rich nickel and amorphous/crystalline molybdenum nitride anchored on a carbon matrix (MoN/Ni@C) as a superior HER electrocatalyst. Owing to the electronic structural modulation of the interfacial synergy of the defects and phase engineering, the MoN/Ni@C exhibits a low HER overpotential of 27 mV at 10 mA cm −2 and a small Tafel slope of 73 mV dec −1 in 1.0 M KOH solution, without any distinct attenuation after 180 h of operation. Density functional theory calculation results demonstrate that the interfacial electron transfer leads to a distorted Ni surface incorporation of the MoN phase, achieving the optimal thermoneutral hydrogen adsorption free energies (ΔG *H ) of Mo and Ni active sites. Meanwhile, the amorphous/crystalline structure in the MoN phase exposes more active sites and promotes structural stability. This work provides new insights into designing heterogeneous interfaces of non-noble-metal-based electrocatalysts with superior HER activities.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Run Yu,Qianqiao Chen,Wenhua Li,Xinyuan Yu,Qin Zhong
Severe photocorrosion and fast photoexcited charges recombination hinder the application of Cu 2 O in photoelectrochemical (PEC) water splitting. In this work, Ni-doped metal-organic frameworks is firstly applied to improve the performance of electrodeposited Cu 2 O. A decorative layer of Ni-doped Cu 3 (BTC) 2 (Ni-CuBTC) was in-suit constructed on Cu 2 O through solvothermal followed by ion-exchange. Cu 2 O/Ni-CuBTC photocathodes increase absorption edge to ∼800 nm, positive shift flat band position to 0.4 V, and decrease Tafel value to 74 mV/dec. These results confirm the decorative layer can extend light absorption, facilitate photoexcited charge separation and transfer, and enhance HER activity. A photocurrent density of −1.51 mA/cm 2 at 0 V RHE is obtained with the decoration of Ni-CuBTC, which is 3.4 times of pristine Cu 2 O photocathode. Here, the PEC water splitting performance of electrodeposited Cu 2 O has been significantly improved with noble-metal-free decorations, which provides a new idea for solving the defects of Cu 2 O based photocathode.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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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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ChemCatChem
·
2022
·Vol. 15
·期 4
·e202201399
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IF 5.497
Changle Fu,Liangliang Feng,Hongyan Yin,Yuhang Li,Guodong Li,Yongqiang Feng,Liyun Cao,Jianfeng Huang,Yipu Liu
Graphical Hierarchized Microflowers for Hydrogen Evoluation Reaction : A novel tactic of synergetic electronic coupling is successfully developed for rationally engineering hierarchical heterostructured electrocatalyst towards hydrogen evolution reaction. The exploration of economical and highly efficient electrocatalysts for hydrogen evolution reaction (HER) is paramount for the development of sustainable hydrogen economy. Herein, a novel three-dimensional (3D) hierarchical microflower electrocatalyst comprised of N-doped carbon-armored Ni 3 P/Ni/VN heterogeneous nanoparticles (Ni 3 P/Ni/VN@NC) is developed by combining a hydrothermal method with in-situ carbonization-phosphating strategy. The unique robust hierarchical structure derived from 3D NiV layered double hydroxide (NiV-LDH) skeleton as precursor provides multidimensional mass and charge transport channels as well as numerous active sites for HER, leading to the improved HER activity. More importantly, the possible electron transfer route of Ni 3 P→Ni→VN is demonstrated due to the charge pumping capability of VN during interfacial electron intercoupling among the tri-component, which endows Ni 3 P/Ni/VN with the favorable absorption of hydrogen-intermediates and thus upgraded HER kinetics over such heterostructure. The resulting Ni 3 P/Ni/VN@NC catalyst exhibits extremely low overpotentials of 81 mV and 134 mV to deliver a current density of 10 mA cm −2 without iR -compensation in alkaline and acidic media, respectively, and maintains continuous operation for over 90 h. This work enlightens the rational design of hierarchical multi-component heterostructured catalysts for efficient hydrogen production.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jiankan Zhang,Fengqi Zhao,Hui Li,Zhifeng Yuan,Ming Zhang,Yanjing Yang,Qing Pei,Ying Wang,Xueli Chen,Zhao Qin
Micron-sized aluminum particles tend to melt into agglomerates, leading to incomplete combustion, two-phase flow losses, and energy decrease of propellants. The higher ignition performance of core–shell Al@Ni makes it a promising candidate fuel with high combustion efficiency. However, little work has been done to study the combustion of Al@Ni in propellants. Here, we report a first attempt to investigate the combustion mechanism of core–shell Al@Ni in the double-based propellant containing high energy explosive HMX , and evaluate its potential as a fuel. Nickel in Al@Ni is determined to play a critical role during its intrinsic combustion and the combustion in propellants. In the condensed phase, the presence of Ni enhances the oxidation process by forming a porous oxide layer on the aluminum surface that promotes oxygen diffusion. Subsequently the phase transition and expansion of Ni break down this oxide layer, leading to the earlier ignition on the burning surface. Upon Al melting, the alloying of Ni and Al accelerates the volume expansion and surface tension reduction of the fuel, giving rise to vigorous melt-dispersion combustion and enhanced energy release. Enhanced thermal feedback and thermal decomposition exotherm combined to increase the burning rate of propellant. The resulting higher flame temperature allows the evaporation of small aluminum droplets into vapor to form smoke oxide productions, further reducing the size distribution of the condensed combustion products (CCPs). This study demonstrates the potential of Al@Ni as an effective fuel for double-based propellants, and provides the insight into its combustion mechanism in HMX-CMDB propellants, which is believed to be important for the development of novel aluminum-based fuels for solid propellants.
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FUEL
·
2023
·
IF 7.4
Dongyang Shen,Jie Wang,Yue Bai,Shuai Lyu,Yuhua Zhang,Jinlin Li,Lin Li,Guanghui Wang
Producing syngas from dry reforming of methane is fascinating but challenging because of coking and sintering. Here, carbonising Ni based catalysts by auto-reduction are fabricated and applied to low-temperature DRM reaction. The catalytic structure–function relationship including the effects of carbonising temperature on carbon structure is investigated and rendered in detail. Ultimately, the carbon-confined catalysts boost DRM reaction at a relatively low temperature of 600 °C and effectively convert greenhouse gases to syngas. The carbon layers obtained by carbonising metal–organic frameworks (MOFs) precursor act as a shell protecting fine Ni nanoparticles (NPs) from reaction-induced reshaping, agglomeration, and coking. This work not only identifies an energy-conserving process for the utilization of greenhouse gases, but also reveals the sintering and coking can be restricted by carbon confinement effect.
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Catalysts
·
2022
·Vol. 12
·期 12
·1525
·
IF 4.501
Sai Che,Na Ta,Fan Yang,Yulong Yang,Yongfeng Li
Rational design and construction of cost–effective electrocatalysts for efficient hydrogen production has attracted extensive research attention worldwide. Herein, we report the construction of a transition metal selenide/carbon composite catalyst featuring uniform NiSe nanoparticles anchored to single Ni atom doped porous carbon structure (NiSe/Ni–N–C) via a facile one–pot pyrolysis of low–cost solid mixtures. NiSe/Ni–N–C exhibits remarkable catalytic performance towards hydrogen evolution reaction (HER) in 1.0 M KOH, requiring a low overpotential of 146 mV to reach a current density of 10 mA cm−2. The unique carbon layer encapsulation derived from the enwrapping of fluid catalytic cracking slurry further renders NiSe/Ni–N–C excellent for long–term durability in electrolyte corrosion and nanostructure aggregation. This work paves the way for the design and synthesis of highly efficient composite HER electrocatalysts.Keywords:NiSe nanoparticle;single atom catalyst;interfacial electronic engineering;hydrogen evolution reaction
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Luping Li,Shuang Cheng,Liyu Deng,Ting Liu,Wenju Dong,Yuxiu Liu,Longjun Huang,Huan Yao,Xu Ji
Alkaline nickel–zinc (Ni–Zn) batteries, as traditional rechargeable aqueous batteries, possess an obvious advantage in terms of energy density, but their development has been hindered by the anode-concerned problems, Zn dendrites, self-corrosion, passivation, deformation, and hydrogen evolution reaction (HER). Herein, to solve these problems, a dual protective strategy is proposed toward the anode using ZnO as an initial active material, including a C coating on ZnO (ZnO@C) and a thin poly(vinyl alcohol) (PVA) layer coating on the electrode (ZnO@C-PVA). In a three-electrode configuration, the reversible capacity can reach 600 mAh g–1 for the ZnO@C-PVA. Using excessive commercial Ni(OH)2 as the cathode, the alkaline Ni–Zn cells exhibit good electrochemical performance: Discharge capacity can be as high as 640–650 mAh g–1 at 4 A g–1 with a Coulomb efficiency (CE) as high as 97–99% after activity, suggesting low self-corrosion and HER. Capacity retention is 97% after 1200 cycles, indicating rather good durability. The discharge capacity is even slightly increased with the increase of charge/discharge current density (≤8 A g–1), implying good rate performance. Additionally, the discharge voltage can reach 1.8 V (midpoint value) at various current densities, reflecting the fast reaction kinetics of the anode. Most importantly, no Zn dendrites and passivation are observed after long-term cycling. The strategy proposed here can solve the anode-concerned problems effectively, exhibiting a high application prospect.
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