Materials Today Communications
·
2025
·
IF 4.5
Jiahua Cheng,Linya Fei,Xiaoqing Zhou,Beibei Lu,Zhihui Zhang,Le Chen,Guojian Ji
UiO-66 and its functionalized derivatives (UiO-66-X, X = -OH, -NO 2 , -NH 2 ) were successfully synthesized via a solvothermal method, and their structural integrity and functionalization were confirmed. Hydrogen adsorption experiments and Grand Canonical Monte Carlo (GCMC) simulations demonstrated that UiO-66-OH exhibited the highest hydrogen adsorption capacity. At 300 K and 1 bar, its experimental adsorption capacity reached 0.0301 wt%, representing increases of 29.18 %, 3.44 %, and 19.92 % compared to UiO-66, UiO-66-NH 2 , and UiO-66-NO 2 , respectively. At 77 K and 20 bar, its simulated adsorption capacity reached 2.352 wt%, surpassing UiO-66-NH 2 (2.229 wt%) and UiO-66-NO 2 (1.927 wt%). This superior performance is attributed to optimized pore structure and enhanced functional group interactions, providing new insights for optimizing hydrogen storage in UiO-66 materials.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Cell Reports Physical Science
·
2022
·
IF 7.832
Jaysree Pan,Qianru Wang,Jianping Guo,Heine Anton Hansen,Ping Chen,Tejs Vegge
Ammonia is a central vector in sustainable global growth, but the usage of fossil feedstocks and centralized Haber-Bosch synthesis conditions causes >1.4% of global anthropogenic CO 2 emissions. While nitrogenase enzymes convert atmospheric N 2 to ammonia at ambient conditions, even the most active manmade inorganic catalysts fail due to low activity and parasitic hydrogen evolution at low temperatures. Here, we show that the [RuH 6 ] catalytic center in ternary ruthenium complex hydrides (Li 4 RuH 6 ) activates N 2 preferentially and avoids hydrogen over-saturation at low temperatures and near ambient pressure by delicately balancing H 2 chemisorption and N 2 activation. The active [RuH 6 ] catalytic center is capable of achieving high yield at low temperatures via a shift in the rate-determining reaction intermediates and transition states, where the reaction orders in hydrogen and ammonia change dramatically. Temperature-dependent atomic-scale understanding of this unique mechanism is obtained with synchronized experimental and density functional theory investigations.
研究领域:
化学
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材料科学
✓ 已验证
DOI
高影响因子
ACS Omega
·
2020
·
IF 2.87
Jianbo Zhao,Jun Wei,Di Cai,Hui Cao,Tianwei Tan
A poly(amino acid)-based approach for scalable synthesis of micro-/mesoporous carbon (PC) with high specific surface area and narrow distribution of micro- and mesopores is presented. Using cross-linked poly aspartic acid as a precursor, PC was obtained by in situ one-step carbonization without the activating agent. The resulting PC had an ultrahigh adsorption capacity for H2 (4.43 wt %) and CH4 (4.49 mmol g–1). This novel method could significantly decrease the wastewater hazards caused by washout of the considerable amount of the activating agent. The PC showed promising application in gas adsorption and storage.
研究领域:
材料科学
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能源存储
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
CORROSION SCIENCE
·
2020
·
IF 6.479
Ning Peng,Libo Liang,Yuqing Wen
This study investigated the adsorption of hydrogen bubbles and tunnel formation on aluminium foil during direct current (DC) electrochemical etching in an electrolyte with and without silicone oil additive. The results indicated that the etched tunnels obtained in the electrolyte containing silicone oil were more uniformly distributed with a more consistent size and length. This was attributed to the additive ability to facilitate the desorption of large bubbles on the aluminium surface, resulting in uniform corroded regions. Moreover, the generated narrow tunnels can accelerate the hydrogen evolution inside the tunnels, resulting in increasing the length of the etched tunnels.
研究领域:
材料科学
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电化学
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金属腐蚀与防护
·
表面工程
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2020
·Vol. 12
·期 14
·3670-3678
·
IF 4.853
Mengjiao Zhang,Youwei Yang,Antai Li,Dawei Yao,Yueqi Gao,Busha Assaba Fayisa,Mei-Yan Wang,Shouying Huang,Jing Lv,Yue Wang,Xinbin Ma
Graphical Cu-based catalyst : In the hydrogenation of ethylene carbonate (EC), nanoflower-like catalysts with high fiber density exhibited nearly 98 % EC conversion when the H 2 /EC ratio was decreased to 60, while the catalyst with solid sphere structure required at least a H 2 /EC ratio of 140. This is attributed to the H 2 -enrichment effect of nanoflower-like morphology with dense fibers, which accelerated the reaction rate and achieved excellent activity at a low H 2 /EC ratio. The hydrogenation of ethylene carbonate (EC) to produce methanol and ethylene glycol (EG) is one of the key steps in the promising route for CO 2 utilization on a large scale. However, the high H 2 /EC ratio in feed (usually as 200∼300) is generally required to achieve favorable catalytic activity, inducing the high cost for H 2 circulation in the industrial application. Here, we report a series of nanoflower-like catalysts with curved fibers and open ends, among which the catalyst with the highest fiber density exhibited nearly 98 % EC conversion, 75 % methanol selectivity and over 99 % EG selectivity when the H 2 /EC ratio was decreased to 60. Combining the characterizations of active species distribution and high-pressure H 2 adsorption, it is demonstrated that the nanoflower-like morphology with dense fibers could remarkably enrich the hydrogen adsorption, consequently, accelerate the reaction rate and present an excellent performance at a low H 2 /EC ratio. These insights may provide instructive suggestions for further design of catalysts for the hydrogenation reactions.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2020
·Vol. 14
·期 5
·857-867
·
IF 3.552
Wei Jun,Zhao Jianbo,Cai Di,Ren Wenqiang,Cao Hui,Tan Tianwei
In addition to the specific surface area, surface topography and characteristics such as the pore size, pore size distribution, and micro/mesopores ratio are factors that determine the performance of porous carbons (PCs) in the fields of energy, catalysis, and adsorption. Based on the mechanism of weight loss of polyaspartic acid at high temperatures, this study provided a new method for adjusting the surface morphology of PCs by changing the cross-linking ratio of the precursor, where cross-linked polyaspartic acid was used as precursor without additional activating agents. N 2 adsorption analysis indicated that the specific surface area of the obtained PCs was as high as 1458 m 2 ·g −1 , of which 1200 m 2 ·g −1 was the contribution of the microporous area and the highest pore volume was 1.13 cm 3 ·g −1 , of which the micropore volume was 0.636 cm 3 ·g −1 . The thermogravimetric analysis results of the precursor, and also the scanning electron microscopy and Brunauer—Emmet—Teller analysis results of the carbonization product confirmed that the prepared PCs presented multilevel pore structure, and the diameters of most pores were 0.78 and 3.97 nm; moreover, the pore size distribution was relatively uniform. This conferred the PCs the ultrahigh hydrogen adsorption capacity of up to 4.52 wt-% at 77 K and 1.13 bar, in addition to their great energy storage and catalytic potential.
研究领域:
材料科学
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能源存储
·
催化
✓ 已验证
DOI
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Qi Peng,Hongwei Zhao,Qilin Yang,Guang Chen,Xinxiu Cao,Shaohui Xiong,Anguo Xiao,Gen Li,Bo Liu,Qingquan Liu
Herein, two types of Fc-based hypercrosslinked polymers (HHCP and DHCP) with high BET surface area (953.9 and 1062.7 m 2 g −1 ) were prepared by direct one-step phenolic polycondensation aiming at high uptake capacity towards H 2 . As expected, the hydrogen uptake values of HHCP and DHCP were notably higher than those of porous polymers with a higher surface area under the same conditions. The maximum H 2 uptake of HCPs at 77 K/1.0 bar are determined to be 2.51 wt % for HHCP and 2.74 wt % for DHCP, respectively. Despite the pore structure playing a determinant role in hydrogen adsorption, the adsorption sites in the polymer framework can be another essential factor to influence the hydrogen adsorption capacity. The interactions between the Fc building block and H 2 are revealed by DFT calculation to fully illustrate the role of Fc in H 2 adsorption. The results indicate that both iron atoms and benzene rings in Fc-based HCPs contribute to the adsorption of hydrogen. Moreover, it is interesting to find that the most stable adsorption site around the Fc building unit is the position directly above the Cp ring. The results in this work may more reasonably explain the phenomenon that the introduction of Fc units could enhance the adsorption of H 2 in many studies, which also provides possible insights into the application of metallocene compounds in H 2 adsorption.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2015
·
IF 4.772
Jinsong Shi,Weibin Li,Dan Li
Porous carbons are important adsorbents for hydrogen. In this work mesoporous carbon material with ultrahigh surface area is prepared with hexagonally packed mesoporous silica (HMS) as template. After a systematic optimization of different synthesis parameters, carbon material with a specific surface area of 2644 m2/g is obtained with resol as carbon precursors, the highest value reported so far for silica-templated mesoporous carbons. The material can be loaded with nickel nanoparticles through addition of nickel chloride hexahydrate into the resol solution. Hydrogen uptake of the nickel-decorated carbon at room temperature and 20 bar reaches 2.66 mmol/g, 78% higher than that of the pristine carbon. Due to the sharp decrease of the specific surface area and pore volume after nickel decoration, the improvement is attributed to effects of nickel nanoparticles.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 44
·13878-13884
·
IF 0
Wuxue Zhao,Xiaodong Zhuang,Dongqing Wu,Fan Zhang,Dominik Gehrig,Frédéric Laquai,Xinliang Feng
Two novel B-π-N based conjugated porous polymers have been successfully synthesized. The full characterization revealed their unique structures, both consisting of alternating π-bridged donor and acceptor subunits. They exhibited high chemical and thermal stabilities, with a weight loss of only 5% at 455 °C and 362 °C, respectively, on the basis of thermogravimetric analysis (TGA) (measured at a heating rate of 20 °C min−1 under flowing N2). Their porous structures were confirmed by transmission electron microscopy (TEM) and nitrogen sorption analyses, revealing high surface areas of up to 1279 m2 g−1. The push–pull electronic structure of such a new type of porous polymer provided rich luminescent properties, solvatochromic emission and electrochemical activities. Furthermore, they showed multifunctions including effective H2 uptake capacities (at 1 bar and 77 K) of 143 cm3 g−1 (1.28 wt%) and 106 cm3 g−1 (0.95 wt%), respectively, fluorescence sensing and collection of fluoride anions.
研究领域:
材料化学
·
物理化学
✓ 已验证
DOI
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Hui Liang,Xihua Du,Jing Li,Limei Sun,Ming Song,Wenjiang Li
The active sites in porous carbon nanotube (CNT) would determine hydrogen storage performance of CNT. Here, we reported an effective, simple and controllable strategy to improve the hydrogen storage property of function group grafted CNT (fg-CNT). N -CNT-M (La 2 O 3 , Ni) would be obtained by the mixture of fg- N -CNT and metallic precursor at calcination of 600 °C. N -CNT-La 2 O 3 has the highest H 2 storage capacity of 7.4 wt%, displaying stable hydrogen adsorption/ desorption cycles for more than 20 times at 100 °C and 18 bar. fg-Ni-CNT-PLLA were formed by electrostatic interactions between C N bond of amide and carbonyl of l -polylactic acid (PLLA). fg- Ni-CNT-PLLA also has H 2 storage capacity of 6.2 wt% at 100 °C and 18 bar. The experiment found that metal ions or PLLA might be dispersed uniformly in CNT by adjusting the ratio of grafted hydroxyl (OH) to acylamino (–CONH 2 ). N -CNT-La 2 O 3 has better hydrogen storage performance than fg-CNT-PLLA because the aggregation of CNT would be caused by the molecular movement of PLLA during hydrogenation and dehydrogenation. This work provides guidance for the development of efficient hydrogen storage materials.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Communications
·
2023
·
IF 3.8
Jin Han,Taolei Qiu,Dan Wu,Yue Zhai,Michael R. Bockstaller,Xiaolin Zhang,Jianchao Zhao
Dimethyl phenol (DMP) oligomers are a side product of industrial poly(phenylethyl ether) (PPE) fabrication and significantly contribute to the environmental burden associated with PPE application. Here, a new process for the upcycling of waste-derived DMP into hyper-crosslinked porous polymer networks through Friedel-Crafts alkylation with p - dichloroxylene as an external crosslink agent is presented. The resulting hypercrosslinked porous polymers exhibited a maximum BET surface area of 740 m 2 /g and displayed and adsorption capacity of 5.9 wt% and 0.85 wt% towards CO 2 (at 1.0 bar, 298 K) and H 2 (at 1.0 bar, 77.3 K), respectively. Form stability of micro- and mesopores was attributed to the rigidity of the aromatic network structure. The results suggest new opportunities for the upcycling of DMP-waste components for applications such as carbon capture that could reduce the negative environmental const associated with the fabrication and application of PPE and related engineering polymers .
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zhewen Ma,Subrata Panda,Qiuyu Zhang,Fengzhan Sun,Darvaish Khan,Wenjiang Ding,Jianxin Zou
For the first time, structure-modified CoS-nanoboxes (CoS-NBs) scaffold as a multifunctional Supporting material has been developed by using a template-consumption method for nanoconfinement of MgH 2 particles within its mesoporous structure (denoted as MgH 2 @CoS-NBs). Microstructural observations via transmission electron microscopy (TEM) reveal the uniform distribution of MgH 2 nanocrystals within the mesoporous networks of CoS-NBs scaffold and the surface decoration of MgH 2 crystals by in-situ formed MgS phase. The peculiar core-shell structured morphology of MgH 2 nanocrystals and the “nano-size effect” notably enhances the thermodynamic properties of MgH 2 through the reduction in hydriding and dehydriding enthalpies (−65.6 ± 1.1 and 68.1 ± 1.4 kJ mol −1 H 2 , respectively). Moreover, the improved hydrogen sorption kinetics can be attributed to the catalytic effect of MgS through reducing the intrinsic kinetic energy barriers for both hydriding and dehydriding (57.4 ± 2.2 and 120.8 ± 3.2 kJ mol −1 H 2 , respectively). The “nano-size effect” of nanoconfined Mg/MgH 2 crystals, the catalyzing effect of MgS and the multifunctional role of CoS-NBs scaffold are likely to be synergistically contributed to the superior hydrogen sorption performances of MgH 2 @CoS-NBs composite, as compared to the pure MgH 2 .
研究领域:
材料科学
·
氢气存储
·
纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）