CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuqiang Ma,Zihang Zhao,Cong Zhang,Yijing Zhang,Chi Zhang,Jiachen Li,Ming Xu,Haixia Ma
Overall water splitting (OWS) involves two important half-reactions, namely hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). However, due to the high theoretical overpotential of OER, OWS needs to be realized with high energy consumption. Using anodic oxidation reaction with lower theoretical potential to replace oxygen evolution reaction (OER) can effectively reduce the energy consumption of overall water splitting (OWS) for hydrogen production. Here, we introduce a new oxidation reaction of green electrosynthesis of energetic materials (EMs) and coupled with OWS. The catalyst was prepared by electrodepositing Pt nanoparticles (Pt NPs) and Pt single atoms (Pt SAs) on MoS 2 nanosheets, which drives highly-efficient hydrogen production of 35.6 mV to drive 10 mA cm −2 . DFT calculations reveal the synergistic mechanism of Pt NPs and Pt SA/MoS 2 substrate for promoting hydrogen production, is that the energy barrier of water dissociation was reduced on the Pt NC sites and the produced H* migrated to the adjacent S sites for Heyrovsky step, while the Pt SA sites served as electron regulator for more thermoneutral H* adsorption on S sites, realizing the synergistic reaction kinetics in MoS 2 /Pt for promoting alkaline HER. Importantly, by integrating the OWS and electrosynthesis of 5,5′-azotetrazole (ZT) EMs, the cell voltage can be significantly reduced to 1.29 V at 10 mA cm −2 , realizing low-energy-consumption for hydrogen production. Meanwhile, the green electrosynthesis of ZT is achieved to avoid the hazardous process of traditional preparation methods. This study presents a new strategy for green electrosynthesis of EMs and low-energy-consumption hydrogen production.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Pengju Su,Qingze Jiao,Hansheng Li,Yongjian Li,Xiufeng Liu,Qin Wu,Daxin Shi,Yun Zhao,Tong Wang,Wei Wang
Composite materials made of bimetallic sulfide quantum dots and carbon nanotubes are promising electrocatalysts due to the large specific surface area and synergistic effect between sulfides and carbon components. In this work, NiCo2S4 quantum dot-modified nitrogen-doped carbon nanotubes (NiCo2S4 QD@NCNTs) are prepared by a two-step solvothermal method, followed by calcination. The dye-sensitized solar cells containing NiCo2S4 QD@NCNTs as a counter electrode (CE) achieve a photoelectric conversion efficiency of 7.65%, which is superior to that of Pt (7.39%), and exhibit good electrochemical stability in iodine-based electrolytes. The notable performance is attributed to the synergistic effect between NiCo2S4 QD and NCNTs. Hence, polypyrrole-derived NCNTs with high electrical conductivity and many uniformly dispersed N-doped species on the surface tightly anchor NiCo2S4 QD through metal–nitrogen bonds (metal–N–C bonds). As a result, the transfer of electrons from the skeleton to the active site is promoted, the agglomeration of NiCo2S4 QD is hampered, and more active sites are available.
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2020
·
IF 4.825
Wenbo Yang,Andrei A. Sukhanov,Jong Hyeon Lim,Xiaoxin Li,Yinshan Meng,Jianzhang Zhao,Haoling Sun,Jin Yong Lee,Gagik G. Gurzadyan,Violeta K. Voronkova
To study the effect of a stable radical on the photophysical properties of a phosphorescent Pt(II) coordination framework and the intramolecular magnetic interaction between radical ligands in the N^N Pt(II) bisacetylide complexes, we prepared a series of N^N Pt(II) bis(acetylide) complexes with oxoverdazyl radical acetylide ligands. The linker between the Pt(II) center and the spin carrier was systematically varied, to probe the effect on the sign and magnitude of the spin exchange interactions between the radical ligands and photophysical properties. The complexes were studied with steady-state and femtosecond/nanosecond transient absorption spectroscopy, continuous-wave electron paramagnetic resonance (EPR) spectroscopy, and density functional theory (DFT) computations. The transient absorption spectral studies show that the doublet excited state of the radicals are short-lived (τD ≈ 2 ps) and nonfluorescent. Moreover, the intrinsic long-lived triplet excited state (τT = 1.2 μs) of the Pt(II) coordination center was efficiently quenched by the radical (τT = 6.9 ps for one representative radical Pt(II) complex). The intramolecular magnetic interaction between the radical ligands through the diamagnetic Pt(II) atom was studied with temperature-dependent EPR spectroscopy; antiferromagnetic exchange interaction (−J S1S2, J = −5.4 ± 0.1 cm–1) for the complex with the shortest radical–radical distance through bridge fragments was observed. DFT computations give similar results for the sign and magnitude of the J values. For complexes with larger inter-radical distance, however, very weak coupling between the radical ligands was observed (|J| < 0.7 cm–1). Our results are useful for the study of the effect of a radical on the photophysical properties of the phosphorescent transition-metal complexes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Qiaoxia Zhang,Weikang Li,Fengyang Zhao,Chang Xu,Gaochao Fan,Qingyun Liu,Xianxi Zhang,Xiao Zhang
An ultrasensitive enzyme-free electrochemical sandwich-type thrombin aptasensor is proposed in this work, with the amplifier of Pt loaded hollow zinc ferrite nanospheres . Silver nanowires& particles (AgNWs&PCs) are used as the substrate materials to decorate the working electrode . Silver particles (AgPCs) are introduced for welding of AgNWs to further improve the electrical performance of the working electrode. The conductive electrode decorated with AgNWs&PCs can provide a substrate for the immobilization of thrombin aptamer 1 (Apt1). Moreover, AgNWs&PCs possess the catalytic activity for H 2 O 2 reduction, contributing to the signal amplification. The prepared Pt loaded hollow zinc ferrite nanospheres with an excellent electrocatalytic activity for H 2 O 2 reduction can also be used to immobilize aptamer 2 (Apt2). Under the optimized condition, the performance of the biosensor is evaluated by amperometry . The proposed thrombin aptasensor has a wide linear detection range from 0.05 pM to 35 nM and a low detection limit of 0.016 pM (S/N = 3), due to the synergistic effect of AgNWs&PCs electrode and the Pt loaded hollow zinc ferrite nanospheres amplifier. This aptasensor displays high sensitivity, good reproducibility and stability, providing a promising platform for the analysis of thrombin.
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2020
·
IF 1.943
Xiaoyan Cao,Hui Yang,Qiulian Wei,Yanting Yang,Mei Liu,Qingyun Liu,Xianxi Zhang
The Pt/NiCo layered double hydroxides nanocomposites (Pt/NiCo-LDH NCs) have been successfully prepared by a one-pot hydrothermal method. Pt/NiCo-LDH was demonstrated to possess an excellent peroxidase-like activity together with a weak oxidase-like activity, evaluating in virtue of rapid catalytic oxidization of 3, 3′, 5, 5′-tetramethylbenzidine (TMB) by H 2 O 2 into a blue oxidation product (oxTMB) only in 30 s. The short response time is very important for designing colorimetric sensors to realize real time detection. The catalytic behaviors of Pt/NiCo-LDH followed the Michaelis-Menten kinetics, possessing a good affinity towards both TMB and H 2 O 2 . The catalytic mechanism of Pt/NiCo-LDH is due to OH radicals from decomposing of H 2 O 2 . Based on the high peroxidase mimetic activity of Pt/NiCo-LDH, a rapid and convenient colorimetric sensing platform for H 2 O 2 and glutathione has been successfully constructed. Under optional conditions, the colorimetric platform shows a sensitive response to H 2 O 2 and glutathione in the linear range of 10–90 mM and 50–500 mM with a limit of detection of 0.76 mM and 3.77 mM, respectively.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 2
·027547
·
IF 3.721
Shuan Zhang,Yueyun Li,Chunyan Zhang,Yilei Jia,Ping Wang,Yunhui Dong,Xinjin Li,Qing Liu,Zengdian Zhao
Herein, urchin-like gold@platinum dendritic nanoparticles supported on molybdenum selenide@molybdenum disulfide (Au@Pt DNPs/MoSe2@MoS2) nanocomposite with multiple signal amplification capabilities was successfully synthesized as the matrix platform of label-free amperometric immunosensor for the quantitative detection of squamous cell carcinoma antigen (SCCA). Au@Pt DNPs/MoSe2@MoS2 consists of Au@Pt DNPs with splendid biocompatibility as well as catalysis and MoSe2@MoS2 with reformative peroxidase activity, which owned enhanced electrocatalysis toward hydrogen peroxide reduction and steady bioconjugation for bioprotein immobilization. Additionally, Au@Pt DNPs/MoSe2@MoS2 possessed satisfactory conductivity to accelerate electron transfer at the electrode interface. With the help of Au@Pt DNPs/MoSe2@MoS2, the immunosensor procured a good linear extent of SCCA detection between 100 fg ml−1 and 100 ng ml−1, reached a lower detection limit than previous reports. Moreover, the immunosensor with good stability and reproducibility achieved the specific detection of SCCA in the mixture containing interferents as well as in the real human serum sample, which testified to the proposed amperometric immunosensor was reliable in clinical detection of tumor biomarkers.
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 3
·638-645
·
IF 8.183
Lei Wenjuan,Li Menggang,He Lin,Meng Xun,Mu Zijie,Yu Yongsheng,Ross Frances M.,Yang Weiwei
The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells. Here, we report a general approach for preparing Pt-M (M = Fe, Co and Ni) bimetallic nano-branched structure (NBs) by a simple high temperature solution-phase synthesis. As-prepared Pt-M NBs show a polycrystalline structure and are rich in steps and kinks on the surface, which promote them favorable bifunctional catalytic properties in acidic electrolytes, specifically in terms of the oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR). Specially, Pt-Co NBs/C catalyst shows 6.1 and 5.3 times higher in specific activity (SA) and mass activity (MA) for ORR than state-of-the-art commercial Pt/C catalysts, respectively. Moreover, it exhibits a loss of 4.0% in SA and 14.4% in MA after 10,000 cycles of accelerated durability tests (ADTs) compared with the initial activities. In addition, we also confirmed the superior MOR activity of Pt-Co NBs/C catalyst in acidic electrolytes. For Pt-M NBs with other alloying metals, the ORR and MOR activities are both higher than commercial catalysts and are in the sequence of Pt-Co/C > Pt-Fe/C > Pt-Ni/C > commercial Pt/C (or PtRu/C). The improved activities and durability can benefit from the morphological and compositional effects. This synthesis approach may be applied to develop bifunctional catalysts with enhanced ORR and MOR properties for future fuel cells designs.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Li Gao,Ubong Jerome Etim,Zhiyuan Shi,Wei Xing,Pingping Wu,Dezhi Han,Peng Bai,Zifeng Yan
A Beta-KIT-6 (BK) micro-mesoporous composite material was assembled using zeolite Beta seed solution as raw material. BK composite contained both zeolite Beta units and three-dimensional cubic Ia3d mesostructure of KIT-6, which served as a catalyst support for hydroisomerization of n-heptane. The composite was characterized by a variety of techniques. Results show that catalyst Pt/HBK using the composite as the support exhibited the highest isoheptanes yield among all catalysts, which is attributed to both appropriate surface acidity and excellent mass transfer properties of Beta-KIT-6 composite. Experimental results verified that the indexed isomerization factor as a general performance descriptor could accurately predict the hydroisomerization performance of support materials.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 8
·H351
·
IF 3.12
Lihui Zhang,Jessie Khungwa,Yue Liu,Ling Li,Xiaohong Wang,Shengtian Wang
A novel electrochemical active electrode based on isopolyacid ion IMo6O245- (IMo6), Pt and graphene oxide (GO) had been fabricated, which was used as a biosensor in double signal amplification platform for simultaneous detection of ascorbic acid (AA), dopamine (DA) and uric acid (UA). Cyclic voltammetry, amperometry and differential pulse voltammetry indicated that a glass carbon electrode modified with Pt/IMo6/GO (Pt/IMo6/GO-GCE) presented higher electrochemical activity toward the oxidation of AA, DA and UA and faster response than those of a bare GCE, GO-GCE, Pt/GO-GCE and IMo6/GO-GCE. As an electrochemical sensor, the Pt/IMo6/GO-GCE showed a wide linear range of 50–4000 μM, 4–750 μM, and 75–300 μM with the limits of detection (S/N = 3) as 6.4 μM, 0.22 μM and 0.72 μM, corresponding to AA, DA and UA, respectively. In addition, the Pt/IMo6/GO-GCE provided a new option in the simultaneous determination of AA, DA and UA in human blood serum with reliable recovery.
✓ 已验证
产品关联
DOI
高影响因子
Materials
·
2018
·Vol. 11
·期 4
·642
·
IF 2.467
Kang Fu,Yang Wang,Ying Qian,Linchang Mao,Junhong Jin,Shenglin Yang,Guang Li
The potential of graphene–multi-walled-carbon nanotube (G-M) hybrids prepared by the one-pot modified Hummers method followed by thermal annealing has been demonstrated by employing one as an electrocatalyst support for oxygen reduction reaction (ORR). N doping effectively modified the electronic structure of the G-M hybrid support, which was beneficial for the uniform distribution of Pt nanoparticles, and ORR activities were further improved. The newly prepared Pt/N-G-M catalyst demonstrated higher electrochemical activity than Pt/G-M and Pt/G catalysts. Even compared with commercial 20 wt % Pt/C (JM20), Pt/N-G-M delivered a better half-wave potential and mass activity. In terms of the durability test, Pt/N-G-M maintained 72.7% of its initial electrochemical active surface area (ECSA) after 2000 repeated potential cycles between 0 and 1.2 V in acidic media in relation to the 44.4% retention for JM20. Moreover, the half-wave potential for Pt/N-G-M showed only a minimal change, significantly superior to the 139 mV of loss for JM20. It is expected that Pt/N-G-M can be the potential candidate as a highly efficient and durable catalyst if utilized in proton exchange membrane fuel cells (PEMFCs).Keywords:oxygen reduction reaction;graphene–multi-walled carbon nanotubes;N doping;proton exchange membrane fuel cells
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Yanfang Wang,Yanjun Guo,Wentao Chen,Qing Luo,Wenli Lu,Peng Xu,Dongliang Chen,Xiong Yin,Meng He
Low-cost catalysts possessing merits of high conductivity and plenty of active sites are highly desirable for the developing of Pt-free counter electrode (CE) in dye-sensitized solar cells (DSCs). In this study, porous sulfur-doped reduced graphene oxide/MoS 2 (S-rGO/MoS 2 ) composites were successfully synthesized via a simple one-step annealing strategy employing CS 2 as sulfur source. Electrochemical measurements revealed that the as-prepared composite presented a superior catalytic activity on the triiodide reduction process, comparable with Pt electrode. Under optimized conditions, a power conversion efficiency of 6.96% was achieved for the N719-sensitized solar cell with a S-rGO/MoS 2 CE, which is very close to that for the device containing a thermally deposited Pt CE (7.35%). The outstanding electro-catalytic activity of composite was attributed to the exposed numerous edges providing much more active sites, and good conductivity resulting from two-dimensional conductive networks of both S-rGO and MoS 2 . This work demonstrated S-rGO/MoS 2 composite as a promising alternative for noble metal Pt in triiodide reduction process and a simple approach of employing two-dimensional nanomaterials as multifunctional materials in photovoltaic for mass application.
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2018
·
IF 13.12
Peng Zhou,Fan Lv,Na Li,Yelong Zhang,Zijie Mu,Yonghua Tang,Jianping Lai,Yuguang Chao,Mingchuan Luo,Fei Lin,Jinhui Zhou,Dong Su,Shaojun Guo
Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). Herein we report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g -C 3 N 4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g -C 3 N 4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m −2 reported to date in carbon-based materials and outstanding H 2 -evolution activity of 174.5 mmol g −1 h −1 per PtSA relative to those on the electron-rich g -C 3 N 4 . The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g -C 3 N 4 via the strong chemical bond between PtSA and the two-coordinated C (C 2C ) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H 2 . This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）