INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Zhoujie Liang,Yu Zhang,Guojie Zhang,Jun Liu,Yajing Cai,Ying Wang,Yuqiong Zhao,Guoqiang Li,Kunlun Bei
In this paper, a series of cobalt catalysts modified by different lanthanide metals were synthesized via co-impregnation method using inexpensive industrial-grade alumina as a support for dry reforming of methane. The effect of lanthanide metals as accelerators of cobalt-based catalysts on catalytic performance and anti-coking properties was mainly investigated. The textural relationships between the catalytic performance and physicochemical properties of cobalt-based catalysts doped with different lanthanide metals were further investigated. Different characterization techniques demonstrate the positive effect of lanthanide metals on the physicochemical properties of catalysts. The results show that the electron transfer between cobalt species and lanthanide metal oxides is significantly enhanced due to the introduction of lanthanide elements. The process generates more active sites, which is favorable for the adsorption and activation of methane. In addition, the abundant medium basic sites and oxygen vacancies on the surface of cobalt-based catalysts with the effect of lanthanides promoted the adsorption and activation of carbon dioxide and the gasification of carbon accumulation, which greatly improved the anti-carbon accumulation performance of the catalysts. Therefore, the prepared cobalt-lanthanum-based catalysts showed the best catalytic effect and have great potential for application.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Zhiyong Zhu,Guanyao Yu,Liangjing Duan,Xiao Liu,Li Wang,Jinglai Zhang
Developing a robust catalyst for CO 2 reduction reaction (CO 2 RR) is critical to achieving a closed carbon cycle. Yet, the process of CO 2 RR still faces enormous challenges, in part because of the lack of highly active, stable, as well as cost-effective electrocatalysts. In this work, we reported an effective and sample strategy to immobilize nickel phthalocyanine (Ni-Pc) molecules on the fruit-peel-derived carbon framework surface (denoted as Ni-Pc/CF and carbon framework denoted as CF) with exceptional CO production performances. Dispersed Ni-Pc molecules on the carbon materials are verified by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman measurements. The obtained Ni-Pc/CF catalyst shows that the high faradaic efficiency (FE) exceeds 95.0 % over a potential of −0.7 to −0.9 V ( vs reversible hydrogen electrode (RHE), V RHE ), the maximum FE (99.1 %) can close to 100 % at −0.8 V, and the excellent stability over a 10 h reaction period. This work offers valuable insights into the immobilization of stabilized, highly dispersed molecule catalysts on carbon materials surfaces for selective reduction of CO 2 to CO.
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Pharmaceuticals
·
2023
·Vol. 16
·期 1
·119
·
IF 4.6
Chen Zhang,Wu Zhong,Ying Cao,Bohao Liu,Xiaojun Tao,Zhuan Li
The treatment of liver cancer remains challenging due to the low responsiveness of advanced cancer to therapeutic options. Sorafenib is the first line chemotherapeutic drug for advanced liver cancer but is frequently associated with severe side effects lead to discontinuation of chemotherapy. We previously developed a specific SIRT7 inhibitor 2800Z, which suppressed tumor growth and enhanced the chemosensitivity of sorafenib. In this study, we constructed polylysine polymer nanoparticles modified with cholesterol and GSH-sensitive PEG (mPssPC) to load sorafenib (SOR) and the SIRT7 inhibitor 2800Z to form dual-loaded NPs ([email protected]) to reduce the toxicity and increase efficacy of sorafenib in liver cancer. The average size of[email protected]NPs was approximately 370 nm and the zeta potential was approximately 50–53 mV. We found that the release of the drugs exhibited pH sensitivity and was significantly accelerated in an acid release medium simulating the tumor environment. In addition,[email protected]NPs inhibited the proliferation and induced apoptosis of liver cancer cells in vitro. An in vivo study further revealed that[email protected]showed high specificity to the liver cancer but low affinity and toxicity to the main organs including the heart, kidneys, lungs, and liver. Our data thus further approved the combination of a SIRT7 inhibitor and sorafenib for the treatment of liver cancer and provided new drug delivery system for targeted therapy.Keywords:polylysine;sorafenib;SIRT7 inhibitor;GSH-sensitive PEG;tumor microenvironment;targeted therapy
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CARBOHYDRATE POLYMERS
·
2022
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IF 10.723
Yucheng Song,Hui Li,Tianhang Shan,Peipei Yang,Songwei Li,Zhong Liu,Chuntai Liu,Changyu Shen
In this study, a composite hydrogel with a low swelling ratio, excellent mechanical properties, and good U (VI) adsorption capacity was developed by incorporating a metal-organic framework (MOF) with a poly (acrylamide- co -acrylic acid)/chitosan (P(AM-co-AA)/CS) composite. The CS chain, which contains NH 2 , reduces the swelling ratio of the hydrogel to 4.17 after 5 h of immersion in water. The coordinate bond between the MOF and carboxyl group on the surface of P(AM-co-AA)/CS improves the mechanical properties and stability of P(AM-co-AA)/CS. The U(VI) adsorption capacity of P(AM-co-AA)/CS/MOF-808 is 159.56 mg g −1 at C 0 = 99.47 mg L −1 and pH = 8.0. The adsorption process is well fitted by the Langmuir isotherm and pseudo-second-order model. The P(AM-co-AA)/CS/MOF-808 also exhibits good repeatability and stability after five adsorption–desorption cycles. The uranium adsorption capacity of the developed adsorbent after one month in natural seawater is 6.2 mg g −1 , and the rate of uranium adsorption on the hydrogel is 0.21 mg g −1 day −1 .
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ADVANCED MATERIALS
·
2022
·Vol. 35
·期 5
·2205262
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IF 32.086
Runyao Zhao,Yiding Wang,Guipeng Ji,Jiajun Zhong,Fengtao Zhang,Meifang Chen,Shengrui Tong,Peng Wang,Zhonghua Wu,Buxing Han,Zhimin Liu
Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers a promising strategy to lower CO 2 emission while producing value-added chemicals. A great challenge facing CO 2 RR is how to improve energy efficiency by reducing overpotentials. Herein, partially nitrided Ni nanoclusters (NiN x ) immobilized on N-doped carbon nanotubes (NCNT) for CO 2 RR are reported, which achieves the lowest onset overpotential of 16 mV for CO 2 -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN x /NCNT affords a CO generation rate of 43.0 mol g −1 h −1 at a low potential of −0.572 V (vs RHE). DFT calculations reveal that the NiN x nanoclusters favor *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO 2 RR overpotential. As NiN x /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm −2 , with total energy efficiency of 62.2%.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Yan Zhang,Chuang Chen,Qiu-Hui Zheng,Zhan-Kuo Guo,Bao-Xia Dong,Yun-Lei Teng
Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped NiII-triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni–S–CT (T = 800, 900, 1000 °C) materials with Ni3S2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i–t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni–S–CT catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni–S–C1000 exhibited the best catalytic activity (FECO of 66.6% and jCO of 1.28 mA/cm2). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni3S2 to illustrate the ECR activity origination. It is the first report on Ni3S2-based catalysts in the application of ECR.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Qiyou,Liu Kang,Hu Kangman,Cai Chao,Li Huangjingwei,Li Hongmei,Herran Matias,Lu Ying-Rui,Chan Ting-Shan,Ma Chao,Fu Junwei,Zhang Shiguo,Liang Ying,Cortés Emiliano,Liu Min
Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO 2 . However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO 2 activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties. In situ attenuated total reflection infrared spectroscopy and theoretical calculations demonstrate that this strategy increases the electron density around the metal centers and facilitates CO 2 activation. As a result, for the electroreduction of CO 2 to CO in aqueous KHCO 3 electrolyte, the cyano-modified catalyst exhibits a turnover frequency of ~22,000 per hour at −1.178 V versus the reversible hydrogen electrode (RHE) and maintains a Faradaic efficiency (FE) above 90% even with a CO 2 concentration of only 30% in an H-type cell. In a flow cell under pure CO 2 at −0.93 V versus RHE the cyano-modified catalyst enables a current density of −300 mA/cm 2 with a FE above 90%.
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 21
·7617
·
IF 4.927
Xiaodong Fang,Xiangguo Wang,Ling Ouyang,Longcheng Zhang,Shengjun Sun,Yimei Liang,Yongsong Luo,Dongdong Zheng,Tairan Kang,Qian Liu,Feng Huo,Xuping Sun
The development of efficient electrochemical seawater splitting catalysts for large-scale hydrogen production is of great importance. In this work, we report an amorphous Co-Mo-B film on Ni foam (Co-Mo-B/NF) via a facile one-step electrodeposition process. Such amorphous Co-Mo-B/NF possesses superior activity with a small overpotential of 199 mV at 100 mA cm−2for a hydrogen evolution reaction in alkaline seawater. Notably, Co-Mo-B/NF also maintains excellent stability for at least 24 h under alkaline seawater electrolysis.Keywords:amorphous Co-Mo-B film;alkaline seawater electrolysis;hydrogen evolution reaction
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高影响因子
International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 4
·2841
·
IF 4.614
Qinghong Li,Huan Yang,Ping Chen,Wenxue Jiang,Fei Chen,Xiaorong Yu,Gaoshen Su
The co-pyrolysis of oily sludge and walnut shell is a reliable method for solid waste treatment and waste recycling. In this paper, a thermogravimetric analysis was used to study the thermodynamics and synergy effect of oily sludge (OS) and walnut shell (WS) at four heating rates (10, 20, 30, and 40 °C/min) in the temperature range from 50–850 °C. Two model-free methods (FWO and KAS) were used to calculate the activation energy. The results showed that the heating rate had no significant effect on the pyrolysis process. The addition of walnut shell improved the pyrolysis process of the samples. Mixture 1OS3WS had a synergy effect, while other blends showed an inhibitory effect. The synergy effect of co-pyrolysis was strongest when the mass ratio of oily sludge was 25%. The activation energy of the Zn-ZSM-5/25 catalyst was the lowest, and the residual substances were the least, indicating that the Zn-ZSM-5/25 was beneficial to the co-pyrolysis of oily sludge and walnut shell. The analysis of catalytic pyrolysis products by Py-GC/MS found that co-pyrolysis was beneficial to the generation of aromatic hydrocarbons. This study provided a method for the resource utilization of hazardous waste and biomass waste, which was conducive to the production of aromatic chemicals with added value while reducing environmental pollution.Keywords:oily sludge;co-pyrolysis;biomass;ZSM-5
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高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 22
·8832-8839
·
IF 4.569
Yihao Gao,Jie Bai,Tianning Zhou,Yaqiong Gong
In recent years, Co-based metal–organic frameworks (Co-MOFs) have received significant research interest because of their large specific surface area, high porosity, tunable structure and topological flexibility. However, their comparatively weak electrical conductivity and inferior stability drastically restrict the application of Co-MOFs in the synthesis of electrocatalysts. In this study, ZIF-67 was grown on nickel foam by a room temperature soaking method, and then Ir–Co(OH)2@ZIF-67/NF was assembled by a hydrothermal method. The prepared Ir–Co(OH)2@ZIF-67/NF nanosheets exhibit remarkable conductivity, larger electrochemical active surface area and wider electron transport channels. Only ultralow overpotentials of 198 mV, 263 mV, and 300 mV were needed for Ir–Co(OH)2@ZIF-67/NF to reach the current densities of 10 mA cm−2, 50 mA cm−2, 100 mA cm−2, meanwhile, no obvious degradation of the current density at 10 mA cm−2 was observed for about 16 h. This work may provide a promising strategy for developing high-performance MOF-derived materials as electrocatalysts for the OER under alkaline conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yuehuan Li,Lang Shi,Yu Mao,Yu Zhang,Hongqing Wang
It is still a challenge for photocatalytic reduction of uranyl and maintaining catalyst stability under aerobic conditions. Herein, a catalyst of sodium–potassium co-doped g-C 3 N 4 (CD-NaK) was obtained to remove Hexavalent Uranium (U(VI)) by photocatalytic reduction under aerobic conditions. And the CD-NaK was characterized by XRD, XPS and other methods. Furthermore, DFT calculations and XRD revealed that Na was doped in-plane while K was doped in-plane and interlayer, enhancing holes and electrons separation performance. Moreover, the removal rate of U(VI) could be achieved nearly 100% after 20 mins of visible irradiation in the presence of air over CD-NaK(30). The photocatalytic activity has the order: CD-NaK(30) > SD-Na > SD-K > CN. Additionally, when the atmosphere of the reaction system was air, the photocatalytic activity of CD-NaK(30) to uranyl was 4.6 times higher than that of pure nitrogen atmosphere in the present of benzyl alcohol, and CD-NaK(30) displayed good reusability and stability with the removal rate > 96% even after five cycles. Interestingly, the effect of the amount of oxygen on catalytic reduction and the role of oxygen were elucidated. Finally, a novel uranyl reduction mechanism has been supposed.
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Advanced Sustainable Systems
·
2022
·Vol. 6
·期 3
·2100321
·
IF 6.737
Pei-dong Wu,Hu Li,Zhen Fang
Bimetallic synergy and carbon–nitrogen doping can contribute to enhanced catalytic activity due to the strong electronic state and unique geometrical structure. In this work, a series of biomass-derived Co-M bimetallic C N doped catalysts (Co-M@Chitosan-X; M = Zr, Ni, Fe, Cu, In; X denotes the molar percentage of M) are prepared via simple oil bath reflow and annealing. The Co-Zr@Chitosan-X catalysts are determined to contain alloys (Co-Zr), metal-carbon bonds (Co-C, Zr-C), metal-nitrogen bonds (Co-N, Zr-N), and metal oxides (Co 3 O 4 , ZrO 2 ) through a series of characterizations, in which graphite-coated alloys and metal oxides are found to be the catalytically active species. The doping of the second metal results in a significant enhancement for the number of active sites in the catalyst, and the d-band center is shifted toward a deviation from the Fermi energy level. Among the tested catalysts, Co-Zr@Chitosan-20 exhibits superior catalytic activity for the reductive amination of biobased levulinic acid to 5-methyl-2-pyrrolidone in 99.3% selectivity and 92.8% yield. This non-noble metal bimetallic synergistic catalytic protocol opens an avenue for efficiently producing biomass-derived nitrogenous chemicals.
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