ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Lingjia Ma,Jiongliang Yuan,Zhaotao Liu,Yiqing Luo,Yuning Su,Kunye Zhu,Zefeng Feng,Huihua Niu,Shuaishuai Xiao,Jianjun Wei,Xu Xiang
The electrocatalytic synthesis of high-value-added urea by activating N2 and CO2 is a green synthesis technology that has achieved carbon neutrality. However, the chemical adsorption and C–N coupling ability of N2 and CO2 on the surface of the catalyst are generally poor, greatly limiting the improvement of electrocatalytic activity and selectivity in electrocatalytic urea synthesis. Herein, novel hierarchical mesoporous CeO2/Co3O4 heterostructures are fabricated, and at an ultralow applied voltage of −0.2 V, the urea yield rate reaches 5.81 mmol g–1 h–1, with a corresponding Faraday efficiency of 30.05%. The hierarchical mesoporous material effectively reduces the mass transfer resistance of reactants and intermediates, making it easier for them to access active centers. The emerging space-charge regions at the heterointerface generate local electrophilic and nucleophilic regions, facilitating CO2 targeted adsorption in the electrophilic region and activation to produce *CO intermediates and N2 targeted adsorption in the nucleophilic region and activation to generate *N ═ N* intermediates. Then, the electrons in the σ orbitals of *N ═ N* intermediates can be easily accepted by the empty eg orbitals of Co3+ in CeO2/Co3O4, which presents a low-spin state (LS: t2g6eg0). Subsequently, *CO couples with *N ═ N* to produce the key intermediate *NCON*. Interestingly, it was discovered through in situ Raman spectroscopy that the CeO2/Co3O4 catalyst has a reversible spinel structure before and after the electrocatalytic reaction, which is due to the surface reconstruction of the catalyst during the electrocatalytic reaction process, producing amorphous active cobalt oxides, which is beneficial for improving electrocatalytic activity.
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CARBOHYDRATE POLYMERS
·
2024
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IF 10.7
Ying Pan,Huifang Sun,Xi Gu,Sujuan Li,Shengtao Yang,Liang Zhang,Hui Mao,Pin Wang,Shasha Yang,Ronghua Yin,Zhili Zuo,Jinhua Zhao
Fucosylated chondroitin sulfate (FCS) from Holothuria mexicana (FCS Hm ) was selected for investigation because of its intriguing branch features. Selective β-eliminative depolymerization and the bottom-up assembly were performed to unravel that FCS Hm consisted of a {D-GlcA-β1,3-D-GalNAc 4S6S } backbone and branches of alternating Fuc S (55 %) and D-GalNAc S -α1,2-L-Fuc S (45 %), the highest proportion of disaccharide branch reported to date. In branches, sulfation could occur at every free -OH site except O-3 of GalNAc, being the most complex and various structure features of natural FCS. Detailed structure-activity relationship analyses showed that FCS Hm and its depolymerized products (>8 kDa) effectively competed with SLe X and PSGL-1 to bind with P-sel at nano-molar level and the inhibition potency increased with Mw increasing. For the structural trisaccharide unit, di-O-sulfation of the Fuc S (Fuc 2S4S and Fuc 3S4S ) was almost 10-fold more potent than mono-O-sulfation (Fuc 4S ). Unexpectedly, higher sulfation of the disaccharide-branched tetrasaccharide unit reduced inhibition. The reversal may attribute to fewer interactions with P-sel by molecular docking study. These results suggested that the specific configuration underpinned the potent inhibition, whereas the size and sulfate number of branches were not the key factors for the specific binding. d Hm F4 (8.0 kDa) potently blocked the platelet-leukocyte aggregates formation, further verifying the potential value in use.
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POLYMER
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2024
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IF 4.1
Chaoying Wang,Jiawei Wang,Zhong Xin
In this work, poly (acrylonitrile-methyl acrylate) [P(AN-MA)] copolymers with controllable molecular weights and narrow polydispersity were successfully synthesized in continuous flow without pre-deoxygenation. A dual-reactor method was designed to prepared P(AN-MA) with higher molecular weight and achieve a high yield from 62.57 % to 70.16 %. To facilitate industrial production of P(AN-MA), pre-mixing stage was added in continuous flow for replacing the ultrasonic mixing process. The characteristic mixing time is 27.80 min and the length of Polyfluoroalkoxy (PFA) tube exceeds 74.625 m for thoroughly mixing. Higher molecular weight P(AN-MA) copolymers possess poorer preoxidation properties such as higher initiation temperature, more concentrated heat release and larger activation energy of cyclization reaction as well as lower extent of stabilization and poorer thermal stability against high-temperature treatment. Moreover, 192 g P(AN-MA) was continuously prepared by the dual-reactor method for 105 min without suffering from notable pressure increase.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Shen Jiafu,Huang Xi,Dai Yu,Zhang Xiaojin,Xia Fan
Low-grade heat is abundant and ubiquitous, but it is generally discarded due to the lack of cost-effective recovery technologies. Ion thermoelectric cells are an affordable and straightforward approach of converting low-grade heat into usable electricity for sustainable power. Despite their potential, ion thermoelectric cells face challenges such as limited Seebeck coefficient and required series integration. Here, we demonstrate that the N-type and P-type conversion of ion thermoelectric cells can be achieved through the phase transition of temperature-sensitive hydrogel containing the triiodide/iodide redox couple. Through the strong interaction between the hydrophobic region of the hydrogel and triiodide, the hydrophobic side selectively captures triiodide and the hydrophilic side repels triiodide, raising the concentration difference of triiodide and thereby increasing the Seebeck coefficient. Specifically, the Seebeck coefficient of the N-type ion thermoelectric cells is 7.7 mV K −1 , and the Seebeck coefficient of P-type ion thermoelectric cells is −6.3 mV K −1 (Δ T = 15 K). By connecting 10 pairs of the N-type and P-type ion thermoelectric cells, we achieve a voltage of 1.8 V and an output power of 85 μW, surpassing the reported triiodide/iodide-based ion thermoelectric cells. Our work proposes a phase transition strategy for the N-P conversion of ion thermoelectric cells, and highlights the prospect of series integrated hydrogel ion thermoelectric cells for low-grade heat harvesting.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Qianqian Song,Yang Chen,Yongjian Xu,Yatao Yan,Qianhui Wu,Fang Guo,Ming Chen,Guowang Diao
Hydrogen energy represents a form of green energy, and the electrolysis of water for hydrogen production is recognized as an efficient method. Current research is primarily focused on the development of catalysts that are both efficient and stable, particularly those capable of functioning consistently across the entire pH spectrum. In this work, Co 9 S 8 /NC co doped with N and P was successfully synthesized through a series of sulfurization, calcination, and phosphating operations using dual ligand Co-ZIF as the precursor. By coating a carbon layer and co doping with nitrogen and phosphorus, the catalytic performance and stability of hydrogen evolution reaction (HER) were significantly improved over the entire pH range. At a fixed current density of 10 mA cm −2 , the overpotential of HER was measured at voltages of 136, 96, and 194 mV in three different pH solutions. Furthermore, the electrocatalyst exhibits remarkable electrochemical stability over extended periods. After 20 h or 2000 cycles of testing, the catalytic activity did not show a significant decrease across the entire pH range, but rather exhibited a relatively sustained constant.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Ziyan Pu,Zengquan Zhu,Xiao-Jun Lv,Yueming Li
Conventional lithium-ion batteries (LIBs) are nearing their theoretical capacity limit, and there is an urgent need to develop energy storage devices with higher energy densities and cycling stabilities. In this work, a hybrid electrode design, which combines the traditional “rocking chair” mechanism and “anion intercalation” mechanism to improve energy density is reported. The hybrid electrode is composed of LiMn 2 O 4 and N,P-doped graphite (NPG) to use both anion and cation storage mechanisms. This design enhances the electrochemical potential windows and the energy density of the fabricated cell. Electrochemical results show that the fabricated cell not only shows a 44.1 % higher capacity than conventional LIBs. It displays a stable cycle life across a wide climate temperature range from − 20 to 25 °C, with a capacity retention rate of 86 % after 600 cycles at 100 mA g −1 . This study demonstrates the critical role of doping graphite with N and P to improve the electrochemical performance of graphite in deep charge/discharge, providing a valuable strategy for developing cathode materials in dual-ion batteries.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Qian Liu,Changdi Wang,Hao Wang,Lu Li,Xingrong Zhang,Ruiyang Zhao,Jishu Han,Lei Wang
Hydrogen energy produced through photocatalytic water splitting is widely recognized as a viable solution to the depletion of non-renewable energy resources and ecological contamination concerns. This work designed and synthesized the MOF-derived hollow octahedral Co x P/MOF-801 p-n heterojunction photocatalyst . According to the result of hydrogen production test, the hydrogen production amount of Co x P/MOF-801-2 could reach 25.31 mmol g −1 under light irradiation for 5 h. The hollow octahedral structure and p-n heterojunction of the photocatalyst helped to enhance the light trapping ability and promote carrier transfer, resulting in improved performance of photocatalytic hydrogen production. To sum up, the design of hollow octahedral Co x P/MOF-801 photocatalyst effectively improved the photocatalytic hydrogen production performance.
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SURFACE REVIEW AND LETTERS
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2018
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IF 0.734
GAO PINGPING,OUYANG CHUN,XIE ZHIYONG,TAO TAO
The Ni-P/TiN coating was used as bipolar plate by electroless plating on Ti. Surface morphology and phase structure of the coatings were characterized by SEM and XRD, respectively. Corrosion resistance of Ni-P and Ni-P/TiN coating was measured in the simulated solution of Proton exchange membrane fuel cells (PEMFCs). The interfacial contact resistance (ICR) was conducted by applied different forces. SEM images indicated that the particles of core–shell structure were formed on the surface of coating on Ti substrate. The core–shell structure was composed of TiN core and Ni-P electroless plating shell. Compared with Ni-P coatings, the Ni-P/TiN coating showed better corrosion resistance behaviors and low ICR (below 10 m Ω cm − 2 under pressure of 200 N/cm 2 ) . TiN particles and distribution of core–shell were in favor of the formation of coating and compact surface morphology. The good conductivity was attributed to the compact surface morphology of coating. The Ni-P/TiN coating showed excellent interfacial conductivity and good corrosion resistance at applied high potential in simulated solution of PEMFCs.
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CARBOHYDRATE POLYMERS
·
2017
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IF 4.811
Ce Gao,Qingda An,Zuoyi Xiao,Shangru Zhai,Bin Zhai,Zhan Shi
Three-dimensional silver/polyethyleneimine/alginate hydrogel beads have been prepared successfully via a facile and simple one-pot assembly method, which can be used efficiently in catalytic hydrogenation reaction of p -nitrophenol under batch and fixed-bed experiment. Polyethyleneimine is used to reduce and limit the growth of nano-silver particle and alginate microsphere is used as the catalyst carrier, leading to form well silver nanoparticles dispersion. Several characterizations were applied to the materials, such as X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy. As-prepared catalysts only spent 120 s finishing reaction at ambient temperature (20% silver load) and stable catalytic performance with high conversion percentage for p -nitrophenol about 90% at 298 K under fixed-bed condition. The relationship between concentration and time was well depicted by Pseudo-first order kinetic model. The catalytic performance for recycled catalyst remained highly efficient, and the conversion efficiency of 96.4% can be maintained after 10 cycles.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2017
·Vol. 32
·期 3
·e4177
·
IF 2.319
Shaohua Wen,Yongfei Li,Weixing Chen,Yaping Lei,Chunyan Luo,Yonggang Hou
A series of L-lactide (LLA), 1,3-trimethylene carbonate (TMC) and glycolide (GA) terpolymers (LTG) of different monomer molar ratios were synthesized by using ring-opening copolymerization. An effective and low-toxic zirconium (IV) acetylacetonate Zr(Acac) 4 was used as catalyst. The viscosity-average molecular weights ( M η ) of obtained polymers were all above 2.2×10 4 g/mol. The chemical structure and viscosity of terpolymers were confirmed by Fourier transform infrared spectroscopy (FTIR), 1 H nuclear magnetic resonance ( 1 HNMR), 13 C nuclear magnetic resonance ( 13 CNMR) and an Ubbelohde viscometer. The thermal and mechanical properties were investigated by means of differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), X-ray diffraction (XRD) and stress-strain measurements. Results suggested that all terpolymers were amorphous and showed good thermal stability. Also it was found that elongation increased with the decreasing of LLA unit. More importantly, terpolymers displayed shape memory property when deformation temperatures were 14-15 °C above T g .
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Yao Yao,Mingli Yin,Junqing Yan,Shengzhong (Frank) Liu
Nanowires assembled sub-WO 3 urchin-like nanostructures have been fabricated via a solvothermal method. The detailed structure and morphology features were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM). The results reveal that the individual nanowires are grown along the [0 0 1] direction, and assembled together to form an urchin-like nanostructure. Sensing performance of the sub-WO 3 was investigated toward alcohol vapor. At room temperature, the sensor devices based on the WO 3−x exhibit significantly higher sensitivity comparing to that of the stoichiometric WO 3 . The superior sensing performance of this WO 3−x sensor is ascribed to the large specific surface area and abundant oxygen vacancies. The obvious enhancement of the gas sensing property can be very useful for the future design and development of room temperature gas sensors for other volatile organic compounds.
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RENEWABLE ENERGY
·
2025
·
IF 9.1
Wenhao Liao,Qinghua Yang,Haiben Jiang,Pengwei Liu
Silver (Ag) and phosphorus (P) doping have been demonstrated to optimize electron density, enhance conductivity, and accelerate electron transfer. Moreover, construction of hollow structures can expose more active sites, significantly improving the performance of catalysts. Therefore, developing P/Ag-doped hollow structures for water splitting is highly promising and meaningful. However, similar studies remain rarely reported. In this work, we designed and synthesized a P-doped Ag 3 [Co(CN) 6 ] hollow cuboid, named as P/Ag@AgCo PBA, aiming to develop an efficient and high-performance water splitting catalyst. Benefiting from its hollow structure and P/Ag co-doping, the optimized P/Ag@AgCo PBA-1 exhibited outstanding catalytic activity. • In the hydrogen evolution reaction (HER), it achieved a current density of 10 mA cm −2 at a low overpotential (η 10 ) of 117 mV with a Tafel slope of 43.6 mV dec −1 . • In the oxygen evolution reaction (OER), the η 10 was 253 mV, and the Tafel slope was 65.3 mV dec −1 . • In the hydrogen evolution reaction (HER), it achieved a current density of 10 mA cm −2 at a low overpotential (η 10 ) of 117 mV with a Tafel slope of 43.6 mV dec −1 . • In the oxygen evolution reaction (OER), the η 10 was 253 mV, and the Tafel slope was 65.3 mV dec −1 . Owing to its excellent HER and OER performance, when employed as both the cathode and anode in overall water splitting, the catalyst required only 1.66 V to reach a current density of 10 mA cm −2 . Furthermore, it demonstrated remarkable catalytic stability over 24 h of continuous operation. We believe this facile and effective etching and heteroatom co-doping strategy offers new opportunities for the development of similar high-performance water splitting catalysts.
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