INORGANIC CHEMISTRY
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2023
·
IF 4.6
Zunpeng Hu,Senjie Dong,Quanfeng He,Zihao Chen,Ding Yuan
Developing electrocatalysts that integrate the merits of the hollow structure and heterojunction is an attractive but still challenging strategy for addressing the sluggish kinetics of oxygen evolution reaction (OER) in many renewable energy technologies. Herein, a 3D hierarchically flexible self-supporting electrode with a hollow heterostructure is intentionally constructed by assembling thin NiFe layered double hydroxide (LDH) nanosheets on the surface of metal–organic framework-derived hollow NiCo2O4 nanoflake arrays (NiCo2O4@NiFe-LDH) for rechargeable Zn–air batteries (ZABs). Theoretical calculations demonstrate that the interfacial electron transfer from NiFe-LDH to NiCo2O4 induces the electronic modulation, improves the conductivity, and lowers the reaction energy barriers during OER, ensuring high catalytic activity. Meanwhile, the 3D hierarchically hollow nanoarray architecture can afford plentiful catalytic active sites and short mass-/charge-transfer pathways. As a result, the obtained catalyst exhibits remarkable OER electrocatalytic performance, showing low overpotentials (only 231 mV at 10 mA cm–2, 300 mV at 50 mA cm–2) and robust stability. When assembling liquid and flexible solid-state ZABs with NiCo2O4@NiFe-LDH as the OER catalyst, the ZABs achieve excellent power density, high specific capacity, superior cycle durability, and good bending flexibility, exceeding the RuO2 + Pt/C benchmarks and other previously reported self-supporting catalysts. This work not only constructs an advanced hollow heterostructured catalyst for sustainable energy systems and wearable electronic devices but also provides insights into the role of interfacial electron modulation in catalytic performance enhancement.
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PubMed
高影响因子
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2023
·Vol. 148
·期 13
·6013-6026
·
IF 4.4
Hu Yinghui,Wang Xuwen,Hao Jingwei,Jiang Shouhang,Zhang Jian,Yang Yulin,Lin Kaifeng,Zheng Jian,Shuai Yong
The excellent thermal decomposition efficiency of ammonium perchlorate (AP) is of great importance for obtaining propellant with fast specific impulse. In this study, four CuM x O y catalysts, including M = Fe, Ni, Co, and Zn, were synthesized and then used for catalyzing AP decomposition and hydroxyl-terminated polybutadiene (HTPB)-based solid propellant combustion. The existed synergistic effect in CuM x O y catalysts improved the catalytic activity and the most active CuZnO catalyst decreased the AP high-temperature decomposition temperature (HTD) from 412.5 to 289.4 °C. Kinetic studies indicated that CuM x O y catalysts inhibited the conversion of N 2 O to a fully oxidized product and decreased the activation energy ( E a ) in HTD to concentrate AP decomposition to significantly decrease the heat loss, thereby increasing their decomposition efficiency. When applying the CuM x O y catalysts in the HTPB (hydroxyl-terminated polybutadiene)-based solid propellant, a faster burning rate and stronger optical emission spectrum were obtained. The CuM x O y catalyst is a potential additive for the preparation of outstanding combustion solid propellants. Graphical abstract
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高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Kai Zeng,Yibing Li,Meng Tian,Chaohui Wei,Jin Yan,Mark H. Rummeli,Peter Strasser,Ruizhi Yang
Crystalline and amorphous structure can entitle a catalyst with high stability and activity, respectively. Oxygen evolution reaction (OER) catalysts, which widely used in water electrolysis and rechargeable Zn-air batteries, often undergo a surface phase reconstruction process and generate amorphous active phases under applied anodic potential. Although widely known, few studies and strategies have been reported to rationally tune OER pre-catalysts for enhanced reaction kinetics. Herein, we report a trimetallic oxides (a/c-NiFeMoO x ) OER per-catalyst with rationally tunable amorphous/crystalline heterostructure degrees by a precise-tuning component strategy. The best a/c-NiFeMoO x electrode exhibits an OER overpotential merely of 256 mV and a small cell-voltage of 1.52 V to reach 10 mA cm –2 for water electrolysis, respectively. It is find that Mo leaching with tailored amorphous/crystalline heterostructure via the rational tuned degree of amorphousness promotes a rapid surface reconstruction of the a/c-NiFeMoO x pre-catalyst to form (oxy)hydroxide active species, whilst operando Raman, ex-situ X-ray photoelectron spectroscopy and density functional theory (DFT) analysis show the ample oxygen vacancies generated by phase transition significantly accelerates the deprotonation of OH* and lower the O* ➝ OOH* free energy for a fast oxygen evolution kinetics. Additionally, the practical application of a/c-NiFeMoO x cathode in rechargeable Zn-air battery delivers a robust long-term cycling (over 840 cycles).
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高影响因子
CORROSION SCIENCE
·
2023
·
IF 8.3
Jingbao Wang,Jingmao Zhao,Mohammad Tabish,Fan Shi,Baomin Fan,Lijun Peng,Qi Cheng
Filiform corrosion (FFC) challenges the application of Zn-Mg-Al coated steel (ZMA-steel). Herein, a self-healing coating loaded with functionalized mesoporous CeO 2 (mCeO 2 ) was developed to suppress FFC for ZMA-steel in saline media. mCeO 2 of large specific area readily accommodated benzotriazole and immobilized on g-C 3 N 4 generating a nanofiller (BTA@mCeO 2 /g-C 3 N 4 ) for epoxy matrix (EP). Strong barrier of lamellar g-C 3 N 4 , releasing BTA from nanofiller and generating Ce cations accounted for the long-term corrosion-resistance and self-healing effect of BTA@mCeO 2 /g-C 3 N 4 /EP system for ZMA-steel. Through taking full advantages of CeO 2 -based nanofiller, this work may provide an intelligent coating to solve FFC of ZMA-steel.
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高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2023
·Vol. 26
·期 24
·e202300303
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IF 2.3
Youyang Xie,Pengtao Sheng,Weili Li,Yanling Li,Songtian Li
Graphical By changing Cu/In molar ratios of Cu−In−Se QDs from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a remarkable red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants. in Cu−In−Se QDs, a significant red-shift occurred from 660 nm to 760 nm when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. These results confirmed the strong effect of the Cu/In and Zn/Cu molar ratios on the intrinsic and dopants states related-transition channels, including the band-edge, conduction band-intragap acceptor, as well as the donor-acceptor. The large structural tolerance of I–III–VI group quantum dots (QDs) to off-stoichiometry allows their photoluminescence properties to be adjusted via doping, thereby enabling application in different fields. However, the photophysical processes underlying their photoluminescence mechanism remain significantly unknown. In particular, the transition channels of CuInSe 2 QDs, which are altered by intrinsic and extrinsic intragap states, remain poorly reported. Herein, we investigated the photophysical processes associated with intragap states via electrochemical and optical techniques by using copper deficient Cu−In−Se QDs as well as Zn doped Cu−In−Se QDs. When the Cu/In molar ratios of Cu−In−Se QDs increased from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants in Cu−In−Se QDs, a significant red-shift occurred (from 660 nm to 760 nm) when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. The Gaussian deconvolution results of the photoluminescence spectra and the band gap derived from absorption spectra by fitting supported the fact that the optical transition channels are dependent on the Cu/In and Zn/Cu molar ratios. After the introduction of the Zn 2+ ions, the alloyed-resultant blue-shift of the emission spectra was observed, primarily due to the enlarged band gap; however, the radiative recombination of prominent intrinsic intragap states is still observed; and only a small proportion of the band-edge exciton undergoes recombination for the sample with low Zn content. Cyclic voltammetry measurements revealed well-defined extrinsic Zn Cu intragap states (Zn substitution on Cu sites) and intrinsic Cu x (x= 1+/2+) states in the band gap. The results presented here provide a better understanding of the varying effects of dopant on photoluminescence in terms of I–III–VI group QDs.
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Energy Storage Materials
·
2023
·
IF 20.4
Zewu Xie,Shaofeng Liu,Canhong Wu,Ruiyi Cai,Na Li,Shaoming Huang
Vanadium-based materials are expected to achieve high-rate capability with high energy density in Zn-ion batteries (ZIBs) due to the layered-structure and multi-electron redox mechanism. However, the high-rate charge/discharge capacity is usually restricted by limited charge storage active sites on material surface and poor electrode kinetics. Herein, homo-interfaces and built-in electric fields were constructed to boost the Zn 2+ diffusion and electron transmission kinetics of NaV 8 O 20 ·xH 2 O (NaVO) nanoflake cathodes, respectively, which cooperated to achieve high-rate charge/discharge capacity in ZIBs. Specifically, firstly, homo-interfacial NaVO nanoflakes were prepared, and then gradient N-doping was introduced from homo-interface to surface of NaVO due to the lower N-doping formation energies of interface than that of surface, which improved electrical conductivity and formed a build-in field to accelerate electron transmission; Moreover, there is a large difference between Zn 2+ concentration in homo-interfaces and surfaces of the N-doped NaVO as the homo-interfaces with lower zinc adsorption energy are more conducive to the adsorption and aggregation of Zn 2+ than that of the surface, which boost Zn 2+ diffusion; Furthermore, numerous micropores were created to shorten ion transport pathways. These structural advantages enabled ultra-fast Zn-storage kinetics and excellent cycling performance of NaV 8 O 20 ·xH 2 O in ZIBs, the reversible capacity can reach 417 mA h g −1 at 0.1 A g −1 , and as high as ∼110 mA h g −1 at 100 A g −1 with capacity retention of 68.4% after 50,000 cycles. Dynamic analysis verifie that high capacitive capacity contributes most to the excellent performance, which can be ascribed to the structural advantages described above. The findings of this study provide new insights for designing Zn-ion storage materials with high-rate capability and long life.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2023
·
IF 2.6
Qiongqiong Luo,Shaoheng Wang,Dehua Cai,Ning Zhang,Dewen Zeng
A ZnSO4 electrolyte solution with impurity salts such as MnSO4 and MgSO4 is often used in zinc hydrometallurgical processes over a wide temperature range. CaSO4·2H2O(s) scaling and fluorine corrosion are two encountered problems in the process. Understanding the CaF2(s) solubility behavior in MSO4 (M = Zn, Mn, Mg) aqueous solutions at various temperatures helps remove Ca2+ and F– ions from the solution. However, CaF2(s) solubility data, especially at temperatures >298 K, have not been published yet. In this work, CaF2(s) solubilities in the CaF2–CaSO4–MSO4–H2O (M = Zn, Mn, Mg) quaternary systems and its subsystems of the CaF2–MSO4–H2O (M = Zn, Mn, Mg) at 348.15 K and the CaF2–CaSO4–MSO4–H2O (M = Zn, Mg) quaternary systems and the CaF2–MgSO4–H2O ternary system at 298.15 K are systematically measured. The results show that the CaF2(s) solubility in the MSO4 (M = Zn, Mn, Mg) aqueous solution of a certain concentration at 348.15 K is considerably higher than that at 298.15 K. At 298.15 and 348.15 K, the salting-in effect of MSO4 (M = Zn, Mn, Mg) on CaF2(s) solubility is enhanced with the order ZnSO4 < MnSO4 < MgSO4. At both temperatures, CaF2(s) solubilities in CaSO4·2H2O(s)- or CaSO4(s)-saturated MSO4 (M = Zn, Mn, Mg) aqueous solutions are generally lower than those in pure MSO4 (M = Zn, Mn, Mg) aqueous solutions. Particularly, the salting-in effect of MgSO4 on CaF2 is so strong that CaF2(s) dissolves completely and is converted to CaSO4·2H2O(s) and MgF2(s) in a concentrated MgSO4 aqueous solution. Hence, this study indicates that high temperatures and high salt concentrations increase the CaF2(s) solubility, making the removal of Ca2+ and F– ions from the system challenging. Further, the existence of impurity salts MnSO4 and MgSO4 makes it more difficult.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Zhikang Deng,Jinyao Zhu,Ping Li,Zhenjie Du,Xuebin Qi,Xi Chen,Rui Mu,Chenyu Zeng,Yongfei Ma,Zulin Zhang
Overuse of tetracycline (TC) has caused serious damage to aquatic environment. Developing sustainable and efficient removal technologies for TC is of great significance to eliminate its ecological risks. In this study, a novel zinc metal organic framework porous biochar composite (Zn-BTC@SBC) derived from sludge was the first time synthesized and employed for adsorptive removal of TC from water. The adsorption process of TC followed the Elovich and Temkin model and the maximum capacity of Zn-BTC@SBC to adsorb TC was 125.9 mg/g. Characterization analysis demonstrated that the greater adsorption capacity of Zn-BTC@SBC was ascribed to its larger surface area, pore volume and abundant oxygen-containing functional groups. The fitting results showed that both chemisorption and physical adsorption predominated the adsorption process of TC on Zn-BTC@SBC. Further material characterization (FTIR and XPS) and density functional theory (DFT) calculations at the molecular level suggested that the good adsorption performance of Zn-BTC@SBC on TC might be due to chemisorption dominated by oxygen-containing functional groups, which included π-π conjugation, H-bonding and electrostatic interaction. And it was a spontaneous, endothermic and randomness increasing reaction. Both ion species/strength and solution pH significantly affected the adsorption capacity of Zn-BTC@SBC for TC. The natural water samples with complex composition (lake and river water) still showed 71.27–76.37 % of TC adsorbed. The used Zn-BTC@SBC was capable of maintaining its stable adsorption capacity by NaOH regeneration. This study demonstrated that Zn-BTC@SBC was a promising practicability in removal of TC and workable approach for sustainable utilization of sludge.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 12
·8556-8563
·
IF 3.3
Zijian Wang,Jiaxin Zhang,Lele Yan,Bo Zhao,Lin Zheng,Haoran Guo,Yuxue Yue,Deman Han,Xianlang Chen,Rongrong Li
4-Chloroaniline (4-CAN) plays an important role in chemical and industrial production. However, it remains a challenge to avoid the hydrogenation of the C–Cl bond in the synthesis process to improve selectivity under high activity conditions. In this study, we in situ fabricated ruthenium nanoparticles (Ru NPs) containing vacancies inserted into porous carbon (Ru@C-2) as a highly efficient catalyst for the catalytic hydrogenation of 4-chloronitrobenzene (4-CNB) with remarkable conversion (99.9%), selectivity (99.9%), and stability. Experiments and theoretical calculations indicate that the appropriate Ru vacancies affect the charge distribution of the Ru@C-2 catalyst, promote the electron transfer between the Ru metal and support, and increase the active sites of the Ru metal, thus facilitating the adsorption of 4-CNB and the desorption of 4-CAN to improve the activity and stability of the catalyst. This study can provide some enlightenment for the development of new 4-CNB hydrogenation catalysts.
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高影响因子
ACS Applied Electronic Materials
·
2023
·
IF 4.7
Qingyue Xu,Wenjing Li,Qi Qi,Ying Guo
Respiration is an important physiological signal that can be used to monitor human health and activity. This study presents a high-performance inorganic composite-based humidity sensor for respiration monitoring. The sensor is composed of a 3D nanostructure of ZnGa-layered double hydroxide (ZnGa-LDH) growing in situ on negatively charged MoS2 wafers, obtained by co-precipitation. By adjusting the MoS2 content, the resulting ZnGa-LDH/MoS2 composite displays a 3D “house of cards” structure with a larger surface area than pure ZnGa LDH or MoS2. The sensor exhibits nearly 3 orders of magnitude impedance change from the humidity range of 11% to 95% RH, fast response/recovery time of 1.5/5 s, hysteresis difference of 2.93%, and long-term stability and high repeatability. The optimized humidity sensor can distinguish between different breathing patterns, as well as the breathing rate/depth of the subject. The conductive mechanism of the material has also been analyzed by combining with the complex impedance curve of the material. This study not only provides an easy approach to adjust the hydrophilic/hydrophobic surface of the materials to control the humidity sensing ability but also develops a humidity sensor that can reflect the breathing conditions of the human body, potentially having applications in respiratory monitoring.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Zexing Wu,Yuxiao Gao,Zixuan Wang,Weiping Xiao,Xinping Wang,Bin Li,Zhenjiang Li,Xiaobin Liu,Tianyi Ma,Lei Wang
Developing multifunctional electrocatalysts toward energy-related reactions could reduce the cost and improve the utilization efficiency of raw materials. Herein, defective CoP decorated with ultrafine Pt nanoparticles (Pt/d-CoP/NPC) with multifunctional electrocatalytic performances is prepared via facile pyrolysis and following chemical reduction process. The as-synthesized Pt/d-CoP/NPC owns high half-wave potential of 0.82 V for oxygen reduction reaction with excellent stability in 0.1 mol/L KOH. Density functional theory calculations demonstrate that the adsorption energy of *OO at Pt/d-CoP/NPC is stronger compared to Pt, yielding higher catalytic activity for ORR. Moreover, the resultant electrocatalyst possesses excellent catalytic activities with low overpotentials toward hydrogen evolution reaction (33 mV in 1 mol/L KOH, 6 mV in 0.5 mol/L H 2 SO 4 and 70 mV in 1 mol/L PBS) and oxygen evolution reaction (320 mV) at 10 mA/cm 2 . Water-splitting and rechargeable Zn-air batteries assembled with the as-synthesized Pt/d-CoP/NPC as electrodes exhibit outstanding activity and long-range stability. Remarkably, sustainable energies and homemade Zn-air battery can efficiently drive the Pt/d-CoP/NPC electrolyzer with sumless hydrogen bubbles generated, verifying the potential applications for renewable energy storage.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Xiao Wang,Tongxin Di,Wei Li,Debao Liu,Xiaohao Sun
Nowadays, Zinc (Zn)-based biocomposites as biodegradable implant materials have been recognized as a promising approach to overcome the insufficient mechanical performance of Zn matrix and to endow the Zn-based materials with biofunctionality. However, the strengthening effect on Zn-based matrix composite remains far from expectation mainly due to the poor interfacial bonding between the reinforcement and Zn matrix, and the relatively coarse grain size of the Zn matrix. Herein, we have developed a novel in situ wetting strategy to ameliorate the interfacial bonding and mechanical performance of Zn-Ag-based composites using cuprous oxide-modified graphene oxide (Cu 2 O-GO) sheets as reinforcement. The enhanced interfacial bonding between GO sheets and Zn matrix owing to the in situ generated ZnO interlayer and the ultrafine microstructure with an average grain size of 360 nm were simultaneously achieved in the hot extruded (HEed) 1 wt%Cu 2 O-GO/Zn-2 wt%Ag biocomposites. Consequently, HEed biocomposites possessed excellent tensile properties, including ultimate tensile strength (UTS) of 344.0 ± 2.4 MPa, yield stress (YS) of 314.0 ± 4.8 MPa, and elongation at failure of 15.5% ± 1.3%. Ultrafine and uniform microstructure of the HEed biocomposites resulted in a relatively uniform corrosion morphology and a degradation rate of 0.195 ± 0.004 mm y −1 in simulated body fluid (SBF) solution. The 2-fold diluted extract of the HEed biocomposites exhibited satisfying cytocompatibility with MC3T3-E1 pre-osteoblast comparable to that of Ti-6Al-4 V ELI alloys. More importantly, the synergistic effect of metallic ions, Ag-rich nanoparticles, and GO sheets contributed to the remarkable antibacterial activity of the experimental biocomposites against both S. aureus and E. coli. These results demonstrated that the 1Cu 2 O-GO/Zn-2Ag biocomposites should be anticipated as a promising biodegradable material for orthopedic applications.
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