JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yang Xiang,Zan Liu,Zhi-lin Cheng
The metal organic framework (MOFs)-derived porous carbon materials with highly dispersed metal active sites were of the exclusive application foreground in many field, such as catalyst, electrochemistry, adsorption desulfurization and so on. However, the loss issue of metal active sites in MOFs frame was indispensable during the high temperature carbonization because of the lower boiling point of many metals, thus fundamentally affecting the atom-scale uniform distribution merit of MOFs-derived porous carbon materials. This work was to provide a novel strategy to address the loss issue of the active metal volatilization in the fabrication of MOFs-derived porous carbon materials. The ZnO nanosheets were pre-grown on the surface of diatomite by using in-situ microwave-assisted preparation, and thereafter the Zn-containing ZIF-8 particles covered the surface of ZnO nanosheets by virtue of the ZnO-induced growth. The results affirmed that the high content Zn-doped porous carbon materials were achieved and the Zn volatilization in MOFs was restrained on account of the occurrence of ZnO on diatomite (DE) surface during the carbonization. The adsorption desulfurization performance of the ZnO/Zn-embedded porous carbon materials/DE (ZnO/Zn/C@DE) was examined by the sulfur-containing compounds in simulated oil. The adsorption desulfurization performance investigation indicated that the ZnO/Zn/C@DE had the optimum adsorption capacities of 45.3 mg/g for benzothiophene and 37.4 mg/g for thiophene. Nonetheless, the competitive adsorption desulfurization finding of toluene in simulated oil showed that the adsorption capacities of ZnO/Zn/C@DE for TH and BT were dramatically descended, suggesting the presence of S-M interaction, wherein S stood for the S atom in a thiophene molecule and their analogs, and M for Zn atoms in porous carbon materials.
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Journal of Cleaner Production
·
2024
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IF 9.7
Wanru Feng,Jingya Zhang,Jianguo Mi,Junsu Jin,Guolei Xiang,Hong Meng,Shisen Xu
The synthesis of structured CO 2 adsorbents with high separation selectivity, strong stability, and low cost to meet industrial needs is very challenging. Here, we synthesized an ultra-stable Zn-MOF (Zn 2 (3-amion-1,2,4-triazolate) 2 (oxalate), Zn 2 (Atz) 2 Ox), and adopted an efficient in-situ growth strategy to produce millimeter-sized spherical Zn 2 (Atz) 2 Ox@AFP (Amino-Functionalization Poly(acrylates), AFP) composite. Due to the heterogeneous crystallization induced by the nanoscale crystal seeds and the confined space of AFP, the three-dimensional (3D) Zn 2 (Atz) 2 Ox bulk crystals transformed into 2D nanosheets with higher CO 2 adsorption efficiency and faster kinetics. Zn 2 (Atz) 2 Ox@AFP has a high affinity for CO 2 (2.05 mmol g −1 at 0.05 bar and 313 K) while exhibiting an inhibitory effect for N 2 (only 0.051 mmol g −1 at 1.0 bar and 313 K), leading to an excellent ideal adsorbed solution theory (IAST) selectivity (2990 for CO 2 /N 2 (5/95, v/v)). Interestingly, Zn 2 (Atz) 2 Ox@AFP exhibits a unique gating effect on CH 4 adsorption, which further extends its application range to natural gas purification. Dynamic breakthrough experiments confirmed that Zn 2 (Atz) 2 Ox@AFP can selectively capture CO 2 in the simulated CO 2 /N 2 (5/95) and CO 2 /CH 4 (5/95) mixed gases.
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LANGMUIR
·
2024
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IF 3.7
Zhe Zheng,Kaiyu Dong,Xiaotong Yang,Qiang Yuan
Metallenes have received sustained attention owing to their unique microstructure characteristics and compelling catalytic applications, but the synthesis of multielement crystalline–amorphous metallenes remains a formidable challenge. Herein, we report a one-step wet chemical reduction method to synthesize composition-tunable crystalline–amorphous heterophase PdMoCrW tetrametallene. As-synthesized PdMoCrW tetrametallene is composed of approximately six to seven atomic layers and has flexible crimpiness, a crystalline–amorphous heterophase structure, and high-valence metal species. Time-dependent experiments show that PdMoCrW tetrametallene follows a three-step growth mechanism that includes nucleation, lateral growth, and atom diffusion, respectively. The novel ultrathin structure, optimized Pd electronic structure, and hydrophilic surface together greatly promote the activity and stability of PdMoCrW tetrametallene in the alkaline oxygen reduction reaction. Pd75.9Mo9.4Cr8.9W5.8/C exhibits excellent mass and specific activities of 2.81 A mgPd–1 and 4.05 mA cm–2, which are 20.07/14.46 and 23.42/16.20 times higher than those of commercial Pt/C and Pd/C, respectively. Furthermore, a Zn–air battery assembled using Pd75.9Mo9.4Cr8.9W5.8/C as a cathode catalyst achieves a peak power density of 156 mW cm–2 and an ultralong durability of 329 h. This study reports an effective strategy for constructing crystalline–amorphous quaternary metallenes to advance non-Pt electrocatalysts toward oxygen reduction reaction (ORR) performance and for a Zn–air battery.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Liang Chen,Jialin Zhao,Jinlong Li,Yan Zhuang,Dongxuan Guo,Shuang Meng,Dantong Zhang,Xue Yang,Guozhe Sui
Bimetallic-organic frameworks and their derivatives have attracted intensive attention in the field of photocatalytic hydrogen production due to their high porosity, distinctive three-dimensional structure, and favorable specific surface area. Despite these advantages, the efficiency of photocatalytic hydrogen production remains unsatisfactory owing to rapid complexation of electron-hole pairs and limited visible light utilization. Herein, in this work, the autogenous CuO–ZnO heterojunction nanoparticles are assembled on the surface of reduced graphene oxide (RGO) by calcining copper-zinc bimetallic-organic frameworks. The autogenous heterojunctions offer numerous active sites and enhance electron transfer at tightly bound heterogeneous interfaces. Furthermore, RGO acts as a co-catalyst or substrate, improving photocatalytic performance with its high surface area and excellent electron transport properties. Consequently, the RGO/CuO–ZnO Z-scheme heterojunction achieves an impressive hydrogen production rate of 479.73 μmol g −1 h −1 , which is 94.06 times higher than that of pristine ZnO. Overall, this work optimizes the potential of metal-organic framework-derived photocatalysts in hydrogen production and offers valuable insights into the effective construction of autogenous heterojunctions.
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Nano-Micro Letters
·
2024
·Vol. 16
·期 1
·1-14
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IF 31.6
Li Bin,Ruan Pengchao,Xu Xieyu,He Zhangxing,Zhu Xinyan,Pan Liang,Peng Ziyu,Liu Yangyang,Zhou Peng,Lu Bingan,Dai Lei,Zhou Jiang
A fluorinated zincophilic covalent organic framework (COF-S-F) with sulfonic acid group (-SO 3 H) is prepared on the surface of Zn anode, which promotes the desolvation of hydrated Zn ions and inhibits the side reactions.
The highly electronegative -F group in COF-S-F promotes fast and uniform transport of Zn ions along the interconnected channels, which contributes to the uniform electrodeposition process of Zn metal.
Zn@COF-S-F symmetric cell achieves a superior stability of 1,000 h and Zn@COF-S-F|MnO 2 cell delivers high specific capacity of 206.8 mAh g −1 at current density of 1.2 A g −1 .
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INDUSTRIAL CROPS AND PRODUCTS
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2025
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IF 6.2
Yao Wu,Jinxin Lan,Lvlv Xu,Jinsen Xu,Jun Wang,Xiaojuan Ma,Shilin Cao
Cotton textiles (CTs) with antibacterial and antiviral activity are of great concern due to the needs of the health and hygiene fields. Herein, chitosan oligosaccharide (COS) and divalent zinc ion Zn (II) were innovatively introduced onto the CTs via esterification and coordination reaction initiated by citric acid (CA) and enabled the CTs with prominent antibacterial and antiviral activity ( Escherichia coli : 100 %, Staphylococcus aureus: 100 % , MS2: 99.9 %). The individual COS and Zn (II) modified CTs showed limited antibacterial performance; only concentrated zinc chloride (at least 10 %) treatment could enable the CTs to have a comparative effect with that of the combined treatment of the COS and Zn (II) (1 %). The sequential COS modification and zinc chloride (2 %) treatment was proved to be the optimum because of the 100 % bacterial inhibition rate benefitting from the dual antibacterial and antiviral mechanism originating from COS and Zn (II). The post treatment with excessive zinc chloride could shift the antibacterial mechanism from the dual to the individual action and therefore postponed to inhibit bacterial propagation. More importantly, the post Zn (II) modification could compensate for the strength loss of cotton cloth caused by the acidic degradation of cellulose. The co-modification affects the color and hydrophobicity of the CTs significantly other than the properties of toughness, softness, slipperiness, and drapeability. This strategy has the advantages of an eco-friendly and simple process, which is a good choice for preparing safe, economical, and efficient antibacterial and antiviral CTs.
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Advanced Science
·
2024
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IF 14.3
Jinxian Feng,Chunfa Liu,Lulu Qiao,Keyu An,Sen Lin,Weng Fai Ip,Hui Pan
Electrolyte plays crucial roles in electrochemical CO 2 reduction reaction (e-CO 2 RR), yet how it affects the e-CO 2 RR performance still being unclarified. In this work, it is reported that Sn-Zn hybrid oxide enables excellent CO 2 -to-HCOO − conversion in KHCO 3 with a HCOO − Faraday efficiency ≈89%, a yield rate ≈0.58 mmol cm −2 h −1 and a stability up to ≈60 h at −0.93 V, which are higher than those in NaHCO 3 and K 2 SO 4 . Systematical characterizations unveil that the surface reconstruction on Sn-Zn greatly depends on the electrolyte using: the Sn-SnO 2 /ZnO, the ZnO encapsulated Sn-SnO 2 /ZnO and the Sn-SnO 2 /Zn-ZnO are reconstructed on the surface by KHCO 3 , NaHCO 3 and K 2 SO 4 , respectively. The improved CO 2 -to-HCOO − performance in KHCO 3 is highly attributed to the reconstructed Sn-SnO 2 /ZnO, which can enhance the charge transportation, promote the CO 2 adsorption and optimize the adsorption configuration, accumulate the protons by enhancing water adsorption/cleavage and limit the hydrogen evolution. The findings may provide insightful understanding on the relationship between electrolyte and surface reconstruction in e-CO 2 RR and guide the design of novel electrocatalyst for effective CO 2 reduction.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
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IF 18.5
Fulong Zhu,Zhengcheng Hu,Wei Guo,Yongzhu Fu
Alkaline zinc-iron flow batteries (ZFBs) have recently attracted renewed attention. However, the critical issues with zinc anodes, such as dendrite formation, side reactions, and labile plating or stripping, have yet to be adequately addressed. Here, an attempt is made to overcome these challenges by designing Boron-doped carbon-felt (B–CF) electrodes rich in electron-deficient sites and defects. The fabricated B–CF provides improved adsorption of negatively charged Zn(OH) 4 2− , robust Zn nucleation sites, and lower Zn nucleation and deposition overpotentials, leading to homogeneous Zn deposition morphology. Uniform Zn deposition enables the prevention of undesirable dendrite growth and parasitic reactions. As a result, the constructed alkaline ZFBs achieve a high average Coulombic efficiency of ≈99.85% and energy efficiency of 88% with uniform Zn deposition during 300 cycles (40 mA cm −2 ). This work expands the understanding of the electrode design strategy for achieving favorable Zn plating/stripping.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Yang Song,Yongduo Liu,Shijian Luo,Yuran Yang,Fadong Chen,Meng Wang,Lin Guo,Siguo Chen,Zidong Wei
Zinc metal is a promising choice as a high-capacity and cost-effective anode for aqueous zinc-based batteries. However, it faces challenges related to low cycling stability and poor reversibility due to parasitic reactions and the growth of zinc dendrites. In this study, a solution is proposed by introducing a conductive Ti 4 O 7 layer on the zinc anode to enhance electrode stability. The Ti 4 O 7 layer serves a dual purpose, effectively preventing spontaneous corrosion of the zinc anode in the electrolyte, thereby inhibiting the hydrogen evolution reaction and the generation of byproducts. Simultaneously, it promotes Zn nucleation and ensures a uniform electric field distribution, resulting in homogeneous Zn plating and stripping compared to using a bare zinc anode. Consequently, the Ti 4 O 7 -coated Zn anode experiences a significant reduction in over-potential, demonstrating long-term stability and dendrite-free behavior. This outcome ensures low polarization potential and high cycling stability in zinc-ion batteries. The work underscores the potential of conductive oxides in the development of stable metal electrodes.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Qi-Hua Yang,Gui-Hua Li,Yu-Chen Ao,Shu-Juan Zhao,Han-Qi Wei,Le Fu,Zhi-Wei Luo,Tian-Liang Zhou,Chu-Jie Wang,Ge-Mei Cai
As a new generation of environmentally friendly halide materials, Cs 3 Cu 2 I 5 shows up the promising application in scintillation, LED, and photoelectric detection fields. However, liquid phase methods cannot produce Cs 3 Cu 2 I 5 on a large scale, and the preparation process is accompanied by serious pollution. Although the ball milling method can solve the problems caused by the liquid phase synthesis method, the Cs 3 Cu 2 I 5 obtained has many surface defects and low luminescence efficiency. In this work, a strategy of doping-assisted ball-milling synthesis using ZnI 2 is proposed. Similar to the chemical preparation of Cs 3 Cu 2 I 5 , the iodine-rich environment during the modified ball milling process can also play a role in repairing surface defects. And it has been demonstrated through experiments and first principles calculations that the distortion of [Cu 2 I 5 ] 3- under ground/excited state can be adjusted through doping Zn into the Cu1 site, the formation barrier of self-trapped excitons is reduced, and the luminous efficiency of Cs 3 Cu 2 I 5 is significantly improved. Subsequently, using the simple hot-pressing method, the representative Cs 3 Cu 2 I 5 :1.0Zn sample was combined with commercially available polypropylene to fabricate Cs 3 Cu 2 I 5 :1.0Zn@PP film. Finally, the potential applications of the newly-developed film in portable and customizable WLED and scintillation fields were explored.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Ye Runping,Ma Lixuan,Mao Jianing,Wang Xinyao,Hong Xiaoling,Gallo Alessandro,Ma Yanfu,Luo Wenhao,Wang Baojun,Zhang Riguang,Duyar Melis Seher,Jiang Zheng,Liu Jian
CO 2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-O V -Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kg cat −1 ·h −1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO 2 with abundant oxygen vacancies can facilitate H 2 dissociation energetically and thus improve CO 2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
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IF 4.7
Jilong Peng,Xunqian Zhang,Rongqing Qin,Fang Lai,Na Shi,Qinggang Ren,Kungang Chai
In the petrochemical industry, efficiently achieving one-step purification of ethylene (C 2 H 4 ) from propylene (C 3 H 6 ) or ethane (C 2 H 6 ) is a highly sought-after yet challenging task. Herein, we present a chlorine-rich Zn-based metal-organic framework (DMOF-1-Cl 2 ) that retains the essential topology of the parent DMOF-1 through the incorporation of 2,5-dichloroterephthalate linkers. The chlorine atoms within the square pores of DMOF-1-Cl 2 , due to their high electronegativity, serve as potential adsorption sites. Gas adsorptive experiments revealed its preferential adsorption of C 3 H 6 and C 2 H 6 over C 2 H 4 at different temperatures. Ideal adsorption solution theory calculation revealed that the selectivity of DMOF-1-Cl 2 for C 3 H 6 /C 2 H 4 and C 2 H 6 /C 2 H 4 reaches 20.8 and 2.2 at 313 K, respectively, outperforming its counterpart (DMOF-1-Br 2 ) and most previously reported adsorbents. Theoretical calculations indicated that the gas molecules are primarily distributed around the chlorine atoms with multiple interactions. Furthermore, dynamic breakthrough experiments fully demonstrated the actual potential for achieving one-step purification of polymer-grade C 2 H 4 , in which DMOF-1-Cl 2 displayed high productivity of 206.1 and 31.6 L kg −1 from C 3 H 6 /C 2 H 4 (2/5, v/v) and C 2 H 6 /C 2 H 4 (1/9, v/v), respectively. Despite the fact that the yield of C 2 H 4 separation from C 2 H 6 /C 2 H 4 mixtures is not extremely high, it still remains at a satisfactory level, demonstrating the practical value and potential of DMOF-1-Cl 2 for industrial applications.
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