MOLECULES
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2023
·Vol. 28
·期 20
·7147
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IF 4.6
Xiafei Gao,Mengyue Gao,Xueping Yu,Xiaoyong Jin,Gang Ni,Juan Peng
The very slow anodic oxygen evolution reaction (OER) greatly limits the development of large-scale hydrogen production via water electrolysis. By replacing OER with an easier urea oxidation reaction (UOR), developing an HER/UOR coupling electrolysis system for hydrogen production could save a significant amount of energy and money. An Al-doped cobalt ferrocyanide (Al-Co2Fe(CN)6) nanocube array was in situ grown on nickel foam (Al-Co2Fe(CN)6/NF). Due to the unique nanocube array structure and regulated electronic structure of Al-Co2Fe(CN)6, the as-prepared Al-Co2Fe(CN)6/NF electrode exhibited outstanding catalytic activities and long-term stability to both UOR and HER. The Al-Co2Fe(CN)6/NF electrode needed potentials of 0.169 V and 1.118 V (vs. a reversible hydrogen electrode) to drive 10 mA cm−2for HER and UOR, respectively, in alkaline conditions. Applying the Al-Co2Fe(CN)6/NF to a whole-urea electrolysis system, 10 mA cm−2was achieved at a cell voltage of 1.357 V, which saved 11.2% electricity energy compared to that of traditional water splitting. Density functional theory calculations demonstrated that the boosted UOR activity comes from Co sites with Al-doped electronic environments. This promoted and balanced the adsorption/desorption of the main intermediates in the UOR process. This work indicates that Co-based materials as efficient catalysts have great prospects for application in urea electrolysis systems and are expected to achieve low-cost and energy-saving H2production.Keywords:hydrogen;urea oxidation;electronic structure;energy-saving;cobalt ferrocyanide
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jundan Tang,Lihua Shen,Kunpeng Zhao,Jiaming Peng,Qili Chen,Chunxia Yu,Yuangang Li,Azhar Abbas,Shan Wang,Zhifang Liu
Nanomaterials-based gas sensors are conducive to online, real-time monitoring and large-scale production due to their simplicity, low energy consumption and miniaturization. Conventional nanomaterial-based (metal oxide semiconductor or two-dimensional nanomaterials) gas sensors are less sensitive (ppm-ppb level). So, it is significantly meaningful to develop new gas-sensing materials. Herein, Ag@sulfur nanosheets (S-NSs) nanocomposite-based sensor is explored for ultrasensitive detection of NH 3 in dry air at room temperature at parts per trillion (ppt) level. Introducing Ag nanoparticles (NPs) on S-NSs, improved electrical conductivity and created more effective adsorption sites, leading to a high response rate of 1.92 for 3 ppt NH 3 . The developed Ag@ S-NSs sensor showed a linear response to NH 3 in the range of 3–70 ppt with correlation coefficient of 0.996. Moreover, the developed Ag@S-NSs sensor showed fast response and recovery time (28/7 s) to NH 3 . The probable sensing mechanism is supposed that the polarization-induction of NH 3 changed of electronic energy level of Ag@S-NSs, and the changed energy is at approximately the same energy level of the Ag@S-NSs itself. Thus, a response signal caused by NH 3 with low concentration can also be felt by Ag@S-NSs sensing materials itself.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Jinxiu Cai,Lingbo Zong,Kaicai Fan,Fuxiang Song,Jianyang Gao,Zumin Wang,Yanan Chen,Lei Wang
Due to energy crisis and environmental pollution, it is urgent to develop efficient and cheap catalysts for hydrogen production from water electrolysis. As a cheaper platinum group metal , Ru , a cheaper platinum group metal, is a highly competitive candidate to Pt because of the similar bond energy of M-H. Herein, TiO 2 @nitrogen-doped carbon composite supported superfine Ru nanoparticles was synthesized by high temperature shock in a Joule furnace using Ti-MOF support (Ru/TiO 2 @NC-J). In the extremely rapid process, MOF was quickly converted into highly conductive nitrogen-doped carbon with tiny TiO 2 dispersed in it, and superfine Ru nanoparticles were generated simultaneously in less than 0.5 s. The obtained Ru/TiO 2 @NC-J displays wonderful HER performance in the wide pH range. In 1.0 M KOH solution, the overpotential was as low as 11 mV at 10 mA cm −2 and a Tafel slope was 39.2 mV dec −1 , which far exceeded the activity of Pt/C and conventional calcined samples as well as most of the recently reported catalysts. The as-developed electrocatalysts also showed excellent stability to accommodate large working current for long term test without obvious activity loss in universal pH range. Experimental investigations suggest that the strong metal-support interaction dominantly facilitate the activity of electrocatalytic hydrogen evolution reaction (HER), and stability of Ru/TiO 2 @NC-J. This strategy provides a new and super-fast methodology to prepare low-budget and high-performance HER catalysts for practical applications.
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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION
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2023
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IF 3.6
Meng-qiu Xia,Jingbao Chen,Liu Liu,Chun-ling Tian,Wang-kai Cheng,Zhiyun Zheng,Xiao-qin Chu
Primary dysmenorrhea is a common disease in women, and oral administration of Ibuprofen (IBU) is associated with first-pass effects and gastrointestinal irritation. Here, we developed ibuprofen-loaded hexagonal liquid crystal (IBU HLC) gel for transdermal administration. In this study, the structure of prepared IBU HLC was characterized using polarizing microscopey (PLM) and small angle X ray diffraction (SAXS). In vitro drug release behavior and percutaneous penetration were investigated, and drug transdermal behavior was observed by confocal laser scanning microscope (CLSM). Finally, the pharmacokinetic profile and tissue distribution were investigated after transdermal administration. The PLM and SAXS results showed that the inner structure of IBU HLC was hexagonal phase. Moreover, in vitro release, skin permeation and CLSM demonstrated that IBU HLC had an excellent sustained-release effect, and a good transdermal penetration effect accompanied by the combination of multiple percutaneous routes. Pharmacokinetic studies indicated that IBU entered the blood circulation through abdominal transdermal administration in small amounts, mainly entering the uterus, and had a certain targeting ability. In conclusion, the IBU HLC gel would be a promising sustained-release preparation for transdermal administration to relieve dysmenorrhea with a significant drug concentration in the uterus.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 40
·18818-18824
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IF 3.3
Yaoxia Yang,Xingwei Guo,Mi Kang,Dangxia Wang,Zhiwang Yang
Developing efficient and inexpensive catalysts for the hydrogen evolution reaction (HER) is critical for the commercial viability of electrochemical sustainable energy technologies. In this study, a La-CoP/Co(OH)2 nanoarray supported on nickel foam (NF) was successfully prepared using the secondary hydrothermal and low-temperature phosphating method. The as-prepared La-CoP/Co(OH)2/NF material exhibited excellent hydrogen evolution performance in 1 M KOH solution. The overpotential of La-CoP/Co(OH)2/NF was 114 mV at the current density of 10 mA cm−2, and the Tafel slope was estimated to be 99 mV dec−1. The decoration of Co(OH)2 nanosheets on La-CoP nanorods with the textured surface not only provides a large surface area and more active sites but also promotes the transfer of electrons between Co(OH)2 and La-CoP, which accelerates the reaction rate and further improve the HER performance of the composite material. Additionally, the fabricated catalyst exhibits good stability and durability in alkaline media. This approach provides a feasible and effective strategy for exploring electrocatalysts with high efficiency and low prices for the electrolysis of water.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 40
·14435-14442
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IF 4
Qihao Wu,Tao Xie,Li Zhang,Hui Ding,Heju Gao,Jiahui Jiang,Guancheng Xu
To achieve broad commercialization of rechargeable metal–air batteries, the development of non-precious metal-based bi-functional oxygen electrocatalysts is critical. In this study, we prepared N,S co-doped porous carbon materials containing Co9S8 nanoparticles (Co9S8/NSC) through a one-step pyrolysis process. The process involved the pyrolysis of a polydopamine (PDA) coated Co-formic acid framework (Co-FF) derived Co3O4 and thiourea. The improved catalyst Co9S8/NSC-1 exhibited satisfactory long-term durability and superior oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity, the half-wave potential (E1/2) of the ORR reached 0.83 V, and the OER overpotential at 10 mA cm−2 (η10) was 300 mV. The zinc–air battery (ZAB) based on Co9S8/NSC-1 assembly had a maximum power density of 102.0 mW cm−2 and the cycle life reached 500 cycles. The material preparation method was simple, environmentally friendly and inexpensive, providing a feasible strategy for the development of non-precious metal-based electrocatalysts.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yunhua Zheng,Huiting Hu,Long Qian,Yao Zhu,Jian Rong,Tao Zhang,Dongya Yang,Fengxian Qiu
Regulating the electrocatalytic hydrogen evolution reaction (HER) performance through defect engineering of the surface of the catalysts is an effective pathway. Herein, cobalt-molybdenum phosphide (CoMoP) nanosheets wrapped molybdenum oxide (MoO 3 ) core–shell nanorods (MoO 3 @CoMoP), as alkaline electrocatalysts with ligand-derived N -doped carbon hybrid and oxygen-vacancies, were synthesized via solvothermal approaches and followed by phosphorization. As expected, the MoO 3 @MoCoP affords efficient HER with a low overpotential ( η ) of 84.2 ± 0.4 mV at 10 mA cm −2 . After phosphorization, not only the MoCoP active species are incorporated into the catalyst, but also the defects sites are achieved. Impressively, the metal–ligand-derived MoCoP are distributed uniformly in the N -doped carbon hybrid matrix, exhibiting well-exposed active sites. Benefiting from the synergy effect of MoCoP active species and oxygen-vacancy, the MoO 3 @MoCoP showed increased conductivity and stability, which can deliver a current density of 10 mA cm −2 over 40 h. MoO 3 @MoCoP exhibits an optimal electronic structure on the surface by charge redistribution at the interface, thereby optimizing the hydrogen adsorption energy and accelerating the hydrogen evolution kinetics. This work paves the way for the design of transition metal electrocatalysts with desirable properties through a promising strategy in the field of energy conversion.
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高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 39
·2301543
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IF 27.8
Qi Wang,Liping Ren,Jie Zhang,Xin Chen,Chunying Chen,Fei Zhang,Shuai Wang,Jie Chen,Jinjia Wei
Low-cost and on-site H 2 O 2 production is desirable for industrial and civilian usage. (Photo)electrochemical H 2 O 2 production is proposed to be a safer, greener, and cheaper strategy for on-site H 2 O 2 production as compared to the conventional anthraquinone process and the direct thermal synthesis. However, the efficiency, selectivity, and durability of the (photo)electrochemical H 2 O 2 production devices are still not satisfactory. Therefore, there is an urgent need to revisit the (photo)electrocatalyst and device designs for (photo)electrochemical on-site H 2 O 2 production, thus to rationalize the research thoughts and provide valuable guidance. This review comprehensively summarizes and discusses the mechanism of two-electron oxygen reduction reaction (2e − ORR) and two-electron water oxidation reaction (2e − WOR) for H 2 O 2 production, and the current research status on the (photo)electrocatalysts and (photo)electrochemical devices. In particular, the pros and cons of the four types of (photo)electrochemical device designs, which are Type I (2e − ORR + oxygen evolution reaction), Type II (2e − ORR + hydrogen oxidation reaction), Type III (2e − WOR + hydrogen evolution reaction) and Type IV (2e − WOR + 2e − ORR), are discussed in detail. Finally, a practical perspective on the future research directions for the on-site (photo)electrochemical H 2 O 2 production based on the technical challenges of this technique is provided.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Ying Yang,Daorui Wang,Lin Gu,Xinruo Luo,Suoying Zhang,Yang Ren,Qi Liu
Endeavors to curb the advanced, cost-efficient and ultra stable electrocatalysts for electrochemical water splitting is critically important for energy conversion. However, their limited electrocatalytic behavior caused by large particles (> 10 nm) has leaded to decreased active surface and interaction with the supporting matrix. Herein, we designed a three-dimensional networked multi-metallic phosphides nanosheet arrays in situ grown on nickel foam (NiCoP-Ni 2 P/NF), within ultrafine nanoparticles ( ca. 2.4 nm) evenly distributed on the skeleton, and the lattice of NiCoP is tensilely strained and contains rich phosphorous vacancies that induce localized compressive strain. Combining experimental investigation and theory calculations on hydrogen/oxygen evolution reaction (HER/OER), the as-established NiCoP-Ni 2 P/NF electrodes realize superior electrocatalytic performance is attributed to the strain effect, that is, tensile strain enhances OER while compressive strain facilitates HER. Moreover, the elaborately fabricated NiCoP-Ni 2 P/NF electrode can be cycled over 300 and 30 hours for hydrogen and oxygen evolution reactions at 10 mA cm –2 , respectively. The concept of lattice strain couples with phosphorous vacancies imposes the rational design of active and ultra stable non-noble metal electrocatalysts for sustainable hydrogen production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yantong Long,Guoliang Zhao,Liuxin Yang,Yuxuan An,Yongjun Xu,Chen Xu
Efficient hydrogen/oxygen evolution reactions (HER/OER) bifunctional catalysts are critical to the overall water splitting efficiency. In this paper, a 1D rod-like structure bifunctional catalyst was firstly prepared, with ultralow Ru (1.19 wt%) loaded into CoNi bimetallic phosphides derived from 1D MOF-74-CoNi nanorods . Due to the strong interface interaction between Co and Ni bimetals which tunes the electronic structure and the Ru loading which increases the number of active sites of the catalyst, the electrocatalytic performance for both HER (8.7mV@10 mA cm −2 ) and OER (179.4mV@10 mA cm −2 ) under alkaline condition were significantly improved. The cell voltage of the full water splitting device assembled by the catalysts was only 1.47 V to achieve 10 mA cm −2 . The rational materials design of 1D rod-like structured bimetallic phosphide catalysts in this work may suggest a new strategy for the preparation of other bifunctional electrocatalysts .
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Weiwei Han,Fan Zhang,Yi He,Chunlin Yu,Lecheng Lei,Xingwang Zhang
Developing highly efficient noble-metal-free bifunctional nanocatalysts for electrocatalytic water splitting is attractive but challenging. Notably, the rational structure engineering could effectively promote electronic transfer and improve the active area. Herein, a free-standing N-doped porous carbon nanosheet arrays encapsulated with metallic Co nanoparticles electrocatalyst (Co@NC-A) for overall water splitting was designed via pyrolysis process followed with acid treatment. The N-doped carbon matrix not only enhances electron mobility and protects the metallic Co nanoparticles from electrolyte corrosion, but also improves the electrochemically active area and facilitates mass transfer. Consequently, the Co@NC-A exhibits superior electrocatalytic performance toward OER ( η 10 = 270 mV) and HER ( η 10 = 162 mV) in 1 M KOH. Moreover, the Co@NC-A as a bifunctional catalyst in overall water splitting could approach 10 mA cm −2 at a cell voltage of 1.66 V and operate stably for 50 h. Combined with the density functional theory (DFT) calculations, the improvement of the HER and OER activities is also attributed to the modified electronic structure with N-doped carbon and the optimized free energy toward the adsorption/desorption of intermediates. This work provides a novel and facile non-precious metal catalyst for water splitting and should be instructive for designing more carbon-based nanocatalysts.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Jianjun Zhu,Xinyu Zheng,Yikai Lu,Huamei Tong,Mengyue Qi,Yu Liu,Di Li,Deli Jiang
The construction of multicomponent coupled interfaces is crucial to designing highly effective and robust bifunctional electrocatalysts for water splitting. Transition metal sulfides are widely applied as efficient catalysts, but building strong coupling interfaces to enhance electrocatalytic properties remains a tremendous challenge. Here, we reported a distinctive heterostructure electrocatalyst consisting of conductive polypyrrole (PPy)-decorated cobalt–molybdenum sulfide (CoS2/MoS2) nanosheets supported on nickel foam (CoS2/MoS2@PPy/NF) using a simple two-step hydrothermal and subsequent electrodeposition approach. Experimental results reveal that the interfacial coupling and synergistic effect between the conductive PPy and CoS2/MoS2 with tunable electronic configuration are favorable for the charge transport and the electronic structure optimization of the coupled interface, where this integrated PPy can improve the conductivity and offer a guarantee for the durability of CoS2/MoS2@PPy/NF. Density functional theory (DFT) calculations verify that electronic interaction and charge redistribution in heterogeneous CoS2/MoS2 can flexibly adjust the interfacial electronic configuration and lower the d-band center. Thanks to the advantages mentioned above, the obtained CoS2/MoS2@PPy/NF exhibits outstanding catalytic properties with the overpotentials of 46 mV for the hydrogen evolution reaction (HER) and 231 mV for the oxygen evolution reaction (OER) at 10 mA cm–2. Remarkably, assembled CoS2/MoS2@PPy/NF || CoS2/MoS2@PPy/NF only acquires 1.52 V at 10 mA cm–2 in 1.0 M KOH with a durability of 50 h. This study affords a significant reference for designing bimetallic sulfide/polymer catalysts toward high-efficiency overall water splitting.
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