Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Zang Ying,Lu Di-Qiu,Wang Kun,Li Bo,Peng Peng,Lan Ya-Qian,Zang Shuang-Quan
Catalysts capable of electrochemical overall water splitting in acidic, neutral, and alkaline solution are important materials. This work develops bifunctional catalysts with single atom active sites through a pyrolysis-free route. Starting with a conjugated framework containing Fe sites, the addition of Ni atoms is used to weaken the adsorption of electrochemically generated intermediates, thus leading to more optimized energy level sand enhanced catalytic performance. The pyrolysis-free synthesis also ensured the formation of well-defined active sites within the framework structure, providing ideal platforms to understand the catalytic processes. The as-prepared catalyst exhibits efficient catalytic capability for electrochemical water splitting in both acidic and alkaline electrolytes. At a current density of 10 mA cm −2 , the overpotential for hydrogen evolution and oxygen evolution is 23/201 mV and 42/194 mV in 0.5 M H 2 SO 4 and 1 M KOH, respectively. Our work not only develops a route towards efficient catalysts applicable across a wide range of pH values, it also provides a successful showcase of a model catalyst for in-depth mechanistic insight into electrochemical water splitting.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 10
·4265-4278
·
IF 3.442
Hu Miao,Yan Aihua,Cui Qiaopeng,Huang Fei,Li Dengke,Li Fan,Huang Ji,Qiang Yinghuai
In this work, nickel sulfide (NiS)/bismuth oxybromide (BiOBr) hybrids were synthesized by a two-step hydrothermal method. Some advanced tools were employed to characterize the crystal phase, morphological evolution, light absorption and photocatalytic performance. Significantly, NiS/BiOBr hybrids exhibited enhanced photocatalytic activity toward rhodamine B (RhB) degradation under visible light irradiation. Comparatively, NS/BOB-3.0 showed the highest degradation rate, over 2.5 times higher than that of pure BiOBr. Furthermore, the retarded recombination rate of photogenerated carriers contributed to the improved photocatalytic performance. The results indicate that hybrids may be a promising method for enhancing the photocatalytic ability of BiOX-based semiconductor.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Zuo Wenhua,Liu Xiangsi,Qiu Jimin,Zhang Dexin,Xiao Zhumei,Xie Jisheng,Ren Fucheng,Wang Jinming,Li Yixiao,Ortiz Gregorio F.,Wen Wen,Wu Shunqing,Wang Ming-Sheng,Fu Riqiang,Yang Yong
Layered transition metal oxides are the most important cathode materials for Li/Na/K ion batteries. Suppressing undesirable phase transformations during charge-discharge processes is a critical and fundamental challenge towards the rational design of high-performance layered oxide cathodes. Here we report a shale-like Na x MnO 2 (S-NMO) electrode that is derived from a simple but effective water-mediated strategy. This strategy expands the Na + layer spacings of P2-type Na 0.67 MnO 2 and transforms the particles into accordion-like morphology. Therefore, the S-NMO electrode exhibits improved Na + mobility and near-zero-strain property during charge-discharge processes, which leads to outstanding rate capability (100 mAh g −1 at the operation time of 6 min) and cycling stability (>3000 cycles). In addition, the water-mediated strategy is feasible to other layered sodium oxides and the obtained S-NMO electrode has an excellent tolerance to humidity. This work demonstrates that engineering the spacings of alkali-metal layer is an effective strategy to stabilize the structure of layered transition metal oxides.
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Nano Research
·
2021
·Vol. 15
·期 4
·2935-2942
·
IF 8.897
Chen Jiayi,Li Xu,Ma Bo,Zhao Xudong,Chen Yantao
The sluggish charge transfer and poor intrinsic activity are the bottlenecks that hamper the further development of electrocatalysts for hydrogen evolution. A novel core-shell heterostructure of Cu 3 P@Ni is fabricated, which is composed of Cu 3 P nanorods covered by metallic Ni. The as-prepared Cu 3 P@Ni exhibits a durable and superior activity toward hydrogen evolution, with an overpotential of 42 mV to deliver 10 mA·cm −2 and a Tafel slope of 41 mV·dec −1 . Charge redistribution is observed after successfully constructing the core-shell heterostructure, leading to the altered electronic structure. The theoretical calculations have manifested that Cu 3 P@Ni exhibits a zero bandgap and optimized adsorption strength of intermediates, which could give rise to the accelerated charge transfer as well as increased intrinsic activity. This work could shed light on the development of novel electrocatalysts with modulated electronic structure for highly efficient hydrogen evolution.
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Science China-Chemistry
·
2022
·Vol. 65
·期 10
·2038-2044
·
IF 10.138
Wang Yanan,Pei Chunlei,Zhao Zhi-Jian,Gong Jinlong
Rational design and performance promotion are eternal topics and ultimate goals in catalyst preparation. In contrast, trial—and—error is still the common method people take. Therefore, it is important to develop methods to intrinsically enhance the performance of catalysts. The most effective solutions are the one from a kinetic perspective based on clear knowledge of the reaction mechanism. This paper describes rate-determining step cognition and modulation to promote CO oxidation on highly dispersed Pt on CeO 2 . The different degrees of metal—support interactions due to variation of hydroxyl density of support could alter the structure of active species and the ability of oxygen activation apparently, further shift the rate-determining step from oxygen activation to oxygen reverse spillover kinetically. The transformation of rate-determining step could enhance the intrinsic activity significantly, and decrease the T 50 approximately 140 °C. The findings of this research exemplify the universal and effective method of performance elevation by rate-determining step modulation, which is promising for application in different systems.
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Nano Research
·
2016
·Vol. 10
·期 1
·238-246
·
IF 8.893
Wang Changhong,Hu Feng,Yang Hongchao,Zhang Yejun,Lu Huan,Wang Qiangbin
Cost-effective electrocatalysts for the hydrogen evolution reaction (HER) play a key role in the field of renewable energy. Although tremendous efforts have been devoted to the search of alternative materials, Pt/C is still the most efficient electrocatalyst for the HER. Nevertheless, decreasing the loading of Pt in the designed eletrocatalysts is of significance. However, with low Pt loading, it is challenging to maintain excellent catalytic performance. Herein, a new catalyst (Pt/NPC) was prepared by dispersing Pt nanoparticles (PtNPs) with an average diameter of 1.8 nm over a three-dimensional (3D) carbon network co-doped with N and P. Because of the high electronegativity of the N and P dopants, PtNPs were uniformly dispersed on the carbon network via high electronic affinity between Pt and carbon, affording a Pt/NPC catalyst; Pt/NPC exhibited superior HER activity, attributed to the down-shift of the Pt d-band caused by the donation of charge from N and P to Pt. The results show that Pt/NPC with an ultralow Pt loading of 1.82 wt.% exhibits excellent HER performance, which corresponds to a HER mass activity 20.6-fold greater than that observed for commercial 20% Pt/C at an overpotential of 20 mV vs. RHE.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 16
·15733-15742
·
IF 2.8
Fu Xiaori,Dionysiou Dionysios D.,Brusseau Mark L.,Zaman Waqas Qamar,Zang Xueke,Lu Shuguang,Qiu Zhaofu,Sui Qian
This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •− ) in the three systems. A gradual increasing contribution of O 2 •− to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl − concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO • oxidation and O 2 •− reaction was proposed.
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Scientific Reports
·
2018
·Vol. 8
·期 1
·1-8
·
IF 4.122
Asokan Vijayshankar,Zhu Dancheng,Huang Wei,Wang Hulian,Gao Wandong,Zhang Ze,Jin Chuanhong
In the present study, a novel method has been carried out to grow tungsten (W) doped molybdenum disulfide (MoS 2 ) on the graphene transferred TEM grid in a chemical vapor deposition (CVD) setup. Tungsten trioxide (WO 3 ) has been used as a source for ‘W’ while ‘Mo’ has been derived from Mo based substrate. Different experimental parameters were used in this experiment. Higher gas flow rate decreases the size of the sample flake and on other side increases the dopant concentrations. The interaction mechanism between Mo, S, W and oxygen (O) have been explored. The influence of oxygen seems to be not avoidable completely which also imposes effective growth condition for the reaction of Mo with incoming sulfur atoms. The difference in the migration energies of Mo, WO 3 , S clusters on the graphene and the higher reactivity of Mo clusters over other possibly formed atomic clusters on the graphene leads to the growth of W doped MoS 2 monolayers. Formation of MoS 2 monolayer and the nature of edge doping of ‘W’ is explained well with the crystal model using underlying nucleation principles. We believe our result provide a special route to prepare W doped MoS 2 on graphene substrate in the future.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 7
·4268-4277
·
IF 2.779
You Yan-bin,Wang Hai-yan,Li Lan,Bai Lin-rui,Dang Zhi-Min
In order to improve the dielectric properties and the thermal conductivity of the PVDF-based composites, the BaTiO 3 @super-short MWCNT (BT@SSCNT) particles were modulated by a SSCNT shell fabricated by MWCNT with the different types (S-MWCNT-1020, S-MWCNT-2040). The average size of these particles is about 300 nm. With the increase in the external diameter of MWCNT, the SSCNT content of the BT@SSCNT particles decreases. However, the sum proportions of which the diameter of the particles is not less than 295 nm have a distinct growth leading to that the distance between the neighboring particles shortens. The dielectric constants of the composites are more than 355 and 1500 (10 3 Hz) at 10 wt% and 60 wt% filler loading, respectively. Compared with the BT@SSCNT/PVDF-1020 composites, the dielectric constants of the BT@SSCNT/PVDF-2040 composites have a more stable frequency dependency in the range of 10 2 to 10 6 Hz. The value of the composite with 10 wt% BT@SSCNT loading maintains more than 250 at 10 6 Hz. The introduction of the shell of SSCNT with larger external diameter can offer the composites a more desirable combined action of dielectric mechanisms, including interfacial polarization and micro-capacitor effect. In addition, the varying SSCNT shells also have evident influence on dielectric loss, breakdown strength, and thermal conductivity. It is worth mentioning that the values of the BT@SSCNT/PVDF-2040 composites are 334 and 0.16 (10 4 Hz), 229 kV mm −1 , and 1.13 W (m K) −1 at 10 wt% filler loading, respectively. This work could extend the strategies for building the core–shell particles to develop dielectric nanocomposites.
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WATER AIR AND SOIL POLLUTION
·
2022
·Vol. 233
·期 12
·1-19
·
IF 2.984
Song Guobin,Tong Liya,Chen Shuhua,Zhang Jing,Zhang Yi,Wang Haonan,Shi Yawei,Sun Ya,Ding Guanghui
In the present study, a series of amino functionalized magnetic multi-walled carbon nanotubes (MMWCNT-NH 2 ) have been prepared by using a facile one-pot solvothermal method and the sorptive removal of anionic dye Congo red (CR) from water was investigated. The composite prepared with triethylenetetramine was found to have higher removal efficiencies due to higher content of amino groups. Characterization analyses confirmed its excellent magnetic separation property and the successful introduction of amino groups on MMWCNTs. The adsorption processes were well fitted by the pseudo-second-order kinetic model, and a three-stage diffusion mechanism had been proved by the intra-particle diffusion model. The maximum adsorption capacities of CR on pristine MMWCNT and MMWCNT-NH 2 -3 were calculated to be 116.7 and 322.7 mg/g at 25 °C, respectively, indicating the great improvement of the adsorption performance after the amino functionalization. The adsorption of CR on MMWCNT-NH 2 -3 performed better under weak acidic conditions due to stronger electrostatic attraction. Several factors, including common anions, typical surfactants, and different organic matters, could suppress the adsorption of CR to varying degrees. Due to the electrostatic attraction and electron donor–acceptor interaction, the selective adsorption of anionic dye could be realized. The prepared MMWCNT-NH 2 -3 exhibited excellent reusability performance with five consecutive cycles. Therefore, MMWCNT-NH 2 -3 prepared in this study could be a promising adsorbent for the sorptive removal of anionic dye from wastewater.
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BioChip Journal
·
2020
·Vol. 14
·期 4
·429-437
·
IF 2.309
Xiong Xiaolu,Zhang Junlin,Wang Zhou,Liu Chenchen,Xiao Wende,Han Junfeng,Shi Qingfan
In order to improve the efficiency of disease diagnosis and environmental monitoring, it is desirable to detect the concentration of proteins and metal ions simultaneously, since the current popular diagnostic platform can only detect proteins or metal ions independently. In this work, we developed a colorimetric microfluidic paper-based analytical device (µPAD) for simultaneous determination of protein (bovine serum albumin, BSA) and metal ions [Fe(III) and Ni(II)]. The µPAD consisted of one central zone, ten reaction zones and ten detection zones in one device, in which reaction solutions were effectively optimized for different types of chromogenic reactions. Fe(III), Ni(II) and BSA can be easily identified by the colored products, and their concentrations are in good accordance with color depth based on the established standard curves. The detection limits are 0.1 mM for Fe(III), 0.5 mM for Ni(II) and 1µM for BSA, respectively. Best of all, we demonstrated the efficiency of the µPAD with accurate detection of Fe(III), Ni (II) and BSA from river water samples within 15 minutes. The µPAD detection is efficient, instrument-free, and easy-to-use, holding great potential for simultaneous detection of cross type analytes in numerous diagnostic fields.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2020
·Vol. 29
·期 5
·1460-1466
·
IF 2.572
Sun Ce,Wang Zanru,Wang Qiong,Cao Jun,Li Wenlong,Tan Haiyan,Zhang Yanhua
In this work, a series of polyurethane/montmorillonite (PU/MMT) nanocomposite films were prepared by in-situ polymerization method. The effect of MMT contents on the properties of the films was investigated using various test methods. MMT enhanced the thermal stability of the films, and the glass transition temperature of PU/MMT films was increased because MMT limited the movement of molecular chains of PU. MMT was well-dispersed in the nanocomposites because the agglomeration of MMT was inhibited by mechanical force. Especially in the PU/4% MMT nanocomposite, MMT showed the best dispersibility. This study showed that the addition of MMT effectively improved the properties of the PU/MMT nanocomposite films.
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