CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·1215-1226
·
IF 2.936
Wang Shiqing,Li Yafei,Lan Xiaocheng,Liu Boyang,Wang Tiefeng
Ni phosphide and Lewis acid–base pair site of Al 2 O 3 were combined as highly efficient catalyst for direct amination of 1-octanol to 1-octylamine. Due to the higher dehydrogenation activity and the site isolation effect, Ni 3 P/Al 2 O 3 -TPP prepared by organophosphorus was 4.0 times more active than Ni/Al 2 O 3 and increased the selectivity to 1-octylamine from 71.4 to 92.8% at 0.4 MPa NH 3 . Graphical Abstract
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Wenli Wu,Lei Feng,Wei Tan,Liqin Han,Qunfeng Yue,Feng Zhang,Xiaoqiang Liang
The rich activated protons and effective proton-conducting paths are of importance to improve conductivities of conductors. Herein, a series of Brönsted acids as proton carrier and proton transfer sites is introduced into the highly stable MOF , contributing to create plentiful hydrogen bonds within frameworks. Consequently, the trifluoromethanesulfonic acid-embedded JUC-1000 ([Cu 24 (BDPO) 12 (H 2 O) 12 ]) displays the relatively highest conductivity of 7.04 × 10 −4 S cm −1 under ∼98% RH and 328 K, ∼16 times that of JUC-1000 (4.47 × 10 −5 S cm −1 ). When TMSA@JUC-1000 (TMSA = CF 3 SO 3 H) blended with chitosan (CS), the proton conductivity of TMSA@JUC-1000/CS-15 is the highest at ∼76% RH and 328 K (1.01×10 −2 S cm −1 ), which is six times higher than that of JUC-1000/CS (1.85×10 −3 S cm −1 ). The CS contains abundant –NH 2 and –OH groups as proton jumping sites, which would activate the –NH– or –OH bonds of JUC-1000 and the acidic groups in Brönsted acids . These would result in an increased content of activated protons and effective formation of H-bonding nets by acid-base interactions. The findings provide valuable insights into the potential application of MOFs materials in energy devices.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaocan Zhang,Jiashu Long,Mengxin Wang,Yiran Liu,Huixiao Ma
Blending metal-organic frameworks to optimize proton transport pathways is one of the strategies to improve the proton conductivity of proton exchange membranes (PEM). In this paper, amino-sulfonic acid bifunctionalized UiO-66 (NUS) by one-pot solvothermal method is synthesized, and sulfonated poly (ether ether ketone)/NUS-X (SPEEK/NUS-X) hybrid membranes are prepared by mixing NUS into SPEEK matrix. Among them, SPEEK/NUS-1.5 has the highest proton conductivity (177.76 mS cm −1 , 70 °C, 100% RH) and maintain a 300 h conductivity stability. And its maximum power density was 423.2 mW cm −2 , exceeding pristine SPEEK by 2.20 times. Compare to the pristine SPEEK membrane, it is interesting to note the disappearance of SAXS scattering peak of SPEEK/NUS-1.5. It is speculated that this phenomenon was caused by the generation of acid-base pairs between –NH 2 and –SO 3 H, and the improved hydrogen bonding network provides more proton transport channels and immobilizes sulfonic acid groups for improved durability. The resultant proton conductivity is stable over 300 h with about 90% retention.
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
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Zean Xie,Zhi Li,Peng Tang,Yangyang Song,Zhen Zhao,Lian Kong,Xiaoqiang Fan,Xia Xiao
Recently, the coordinatively unsaturated metal-O Lewis acid-base pairs of metal oxides are found to be able to activate the C–H bond of light alkane efficiently. For the inert crystal Al 2 O 3 , we found that the surface oxygen vacancy amount of Al 2 O 3 can be controlled by pretreatment of CO reduction, and the nearby coordinatively unsaturated Al-O (Al cu -O) pairs can effectively catalyze propane dehydrogenation (PDH). The C 3 H 6 formation rate of γ/δ-Al 2 O 3 is in line with the concentration of oxygen vacancies. The experiments and DFT calculations illuminate the importance of oxygen vacancy on the surface of Al 2 O 3 for PDH reaction. The consumption of lattice oxygen reduces the one coordination number of the bonding Al, the formed Al cu -O as defective acid-base pairs, can be an effective way to tune the adsorption energy of the intermediates and the barriers of key steps (the first C H activation and H 2 formation) to enhance the performance of PDH through both site-dependent concerted and stepwise mechanisms.
研究领域:
催化化学
·
材料科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Haifan Wang,Menglei Yuan,Jingxian Zhang,Yiling Bai,Ke Zhang,Bin Li,Guangjin Zhang
Ammonia (NH 3 ) synthesis at mild conditions by electrocatalytic nitrogen reduction (eNRR) has received more attention and has been regarded as a promising alternative to the traditional Haber–Bosch process. Lewis acid-base pairs (LPs) can chemisorb and react with nitrogen by electronic interaction, while the tuning of the microenvironment near electrode can hinder hydrogen evolution reaction (HER) thus improving the selectivity of the eNRR. Herein, the FeOOH nanorod coupled with LPs on the surface (i.e., Fe, Fe–O) was synthesized, which could effectively drive eNRR. Meanwhile, polyethylene glycol (PEG) was introduced to serve as a local non-aqueous electrolyte system to inhibit HER . The prepared FeOOH-150 catalyst achieved outstanding eNRR performance with an NH 3 yield rate of 118.07 μg h −1 mg cat −1 and a Faradaic efficiency of 51.4 % at −0.6 V vs. RHE in 0.1 M LiClO 4 + 20 % PEG . Both the experiment and DFT calculations revealed that the interaction of PEG with Lewis base sites could optimize nitrogen adsorption configuration and activation.
研究领域:
化学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FlatChem
·
2023
·
IF 6.2
Shao-Zhen Luo,Zhi-Hua Fu,Jian-Ze Xiao,Xiao-Liang Ye,Qian Liu,Guan-E Wang,Gang Xu
Acid-base pairs synergistic strategy is one of the most effective ways to improve the proton conductivity of materials at low humidity. However, the random distribution of acid or base functional groups on the surface of the materials are difficult to form long-range ordered proton transfer channels, which hinders the proton conductivity. Herein, two organic metal chalcogenides (OMCs), Ag(SPh-NH 2 ) and Ag(SPh-COOH) nanosheets were self-assembled into composite membranes by vacuum filtration. Benefiting from the long-range ordered acid-base functional groups on the surface of OMCs, the proton conductivity was significantly enhanced. As a result, the proton conductivity of the Ag(SPh-NH 2 )/Ag(SPh-COOH) composite membrane is greatly improved at a low humidity condition of 45% RH, reaching the level of the single membrane at high humidity. In addition, the proton conductivity of Ag(SPh-NH 2 )/Ag(SPh-COOH) composite membrane is 47 times higher than that of Ag(SPh-NH 2 ) membrane and 10 times higher than that of Ag(SPh-COOH) membrane under high-temperature hydration state. Collectively, this study broadens the avenue for designing proton-conducting materials that can work under low humidity conditions.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2021
·
IF 7.132
Jiaxin Liang,Shuxian Ye,Wenjing Wang,Congxiao Fan,Shuanjin Wang,Dongmei Han,Wei Liu,Yan Cui,Limin Hao,Min Xiao,Yuezhong Meng
Bulk terpolymerization of carbon dioxide and phthalic anhydride with propylene oxide is successfully carried out using metal-free and economical Lewis pairs under mild conditions. A series of commercial organic bases are coupled with triethyl borane (TEB) as Lewis pairs to optimize the activity and the results show that the TEB/ bis(triphenylphosphine)iminium chloride (PPNCl) pair exhibits relatively high activity and selectivity. The impact of the molar ratio of TEB to organic bases, reaction temperature and CO 2 pressure as well as the catalyst loading on the activity and selectivity of the copolymerization are investigated. Particularly, the turnover frequency reaches 164 h −1 with a TEB/PPNCl molar ratio of 2/1 at 80 °C. To our delight, the poly(ester- co -carbonate)s with random or block structures can be simply tuned by choosing different organic bases coupled with TEB. In these cases, the resultant terpolymers with comprehensive properties can be readily synthesized. As expected, the incorporation of phthalic anhydride effectively modifies the thermal and mechanical properties of commercial poly(propylene carbonate) (PPC). Terpolymers named as PPC-P with 43 mol% aromatic polyester moieties displays a glass transition temperature ( T g ) of 47 °C, about 9 °C higher than that of commercial PPC, and gives a tensile strength higher than 37.6 MPa. To our delight, the synthesized PPC-P exhibits satisfactory degradation speed under standard composting condition compared with commercial PBAT and PPC.
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
ACS Catalysis
·
2025
·
IF 13.1
Zean Xie,Kemeng Song,Yu Ren,Liyu Hou,Runqi Hu,Jianmei Li,Qi Shi,Dong Li,Wencui Li,Xiaoqiang Fan,Lian Kong,Xia Xiao,Zhen Zhao
Recently, some traditional oxide supports, such as nano TiO2 and ZrO2 with high surface energy, have been found to be partially reduced to generate oxygen vacancies and coordinatively unsaturated metal (Mcu) cations as efficient active sites for nonoxidative propane dehydrogenation (PDH). However, the primary challenge in their industrial applications is rapid deactivation because of coke, over-reduction, and aggregation under the reaction conditions of high temperature and reducible atmosphere. Herein, we reported that cost-effective and environmentally friendly Zr-doped TiO2 (TixZr1) prepared by a simple coprecipitation method can be used as a highly efficient and stable catalyst for PDH. Ti3Zr1 exhibited the C3H6 formation rate [r(C3H6)] of 0.6 mmol g–1 min–1 at 550 °C, which was 17 times that of pure TiO2, and a deactivation constant (Kd) 2.8 times lower than that of commercial TiO2. Moderate Zr doping promotes the generation of surface active lattice oxygen, which can be reduced at a relatively low temperature to form oxygen vacancies and Ti(Zr)cu–O acid–base pairs as the active sites for PDH, and their number is in line with r(C3H6) of TixZr1 catalysts. With the increase of the Zr doping amount, the bulk crystal phase of TixZr gradually transforms from Zr-doped anatase TiO2 to TiZrO4 via Ti2ZrO6 with enhanced thermostability, which can inhibit over-reduction and aggregation of the nano-oxide.
研究领域:
化学工程
·
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 31
·16079-16088
·
IF 7.443
Yongheng Yin,Wanyu Deng,Hongyan Wang,Anping Li,Chongbin Wang,Zhongyi Jiang,Hong Wu
Hollow mesoporous silica microspheres with a uniform pore size and a large surface area are synthesized and functionalized by three kinds of amino acids with different acid–base pairs, including sulfonic acid–amino groups (HMS-Cys), phosphoric acid–amino groups (HMS-Phos) and carboxylic acid–amino groups (HMS-Asp). The incorporation of these microspheres into a Nafion matrix enhances the water uptake and adjusts the organic–inorganic interface and hydrophilic ionic domains inside the membranes. Microspheres with a hollow mesoporous structure endow the membranes with strong water retention ability. The proton conductivities of hybrid membranes are more than 8 times higher than that of recast Nafion at 40 °C and 20% RH after 90 min of testing. The acid–base pairs within the membranes work as proton donors and acceptors, and the retained water molecules are used as hydrogen-bonded bridges, which reduce the energy barrier for proton conduction. At the filler content of 4 wt%, the HMS-Cys embedded membrane shows the highest proton conductivity of 1.19 × 10−1 S cm−1 (30 °C, 100% RH). In addition, hybrid membranes incorporated with amino acid functionalized HMS show small reliance on humidity. The proton conductivities of all the hybrid membranes are ∼5.29–11.1 times higher than that of the recast Nafion under 26.1% RH and 80 °C.
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
ChemCatChem
·
2022
·Vol. 14
·期 7
·e202101728
·
IF 5.497
Shiqing Wang,Xiaocheng Lan,Boyang Liu,Babar Ali,Tiefeng Wang
Graphical Octylamine synthesis : Ni x Fe 1 /Al 2 O 3 was used as catalyst for 1-octanol amination and provided the highest yield among the reported nonprecious metal catalysts. The generation of Ni−FeO x interactions provided sufficient Fe 2+ /Fe 3+ −O 2− sites for the activation of 1-octanol. Meanwhile, the cooperation between Ni site and Lewis acid-base pairs significantly enhanced the amination of 1-octanol to 1-octylamine. The synthesis of 1-octylamine, a primary platform molecule, remained a great challenge in catalysis. In this work, Ni x Fe 1 /Al 2 O 3 was used for direct amination of 1-octanol to 1-octylamine. Catalyst evaluation indicated that the promotion effect of Fe/Ni ratio on the catalytic amination activity followed a volcano curve while the selectivity to 1-octylamine was positively correlated with the Fe loading. Compared with the Ni/Al 2 O 3 catalyst, the amination activity was increased by 2.8 times by optimizing the Fe/Ni ratio to 0.33, and the selectivity to 1-octylamine was increased from 84.0 % to 96.3 % when increasing the Fe/Ni ratio from 0 to 1. Based on catalyst characterizations, the good performance of Ni x Fe 1 /Al 2 O 3 was ascribed to the combined modification effect of the NiFe alloy and Ni−FeO x interface. The FeO x species enriched on the Ni particle surface provided sufficient Fe 2+ /Fe 3+ −O 2− sites for the activation of 1-octanol, and the cooperation between Ni sites and Lewis acid-base pairs enhanced the amination of 1-octanol to 1-octylamine. This work sheds new light on the design of Ni-based catalysts without using a noble metal for primary amine preparation.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xianqiang Gao,Lulu Cao,Ying Chang,Zhimin Yuan,Shuxin Zhang,Shujun Liu,Mengting Zhang,Hai Fan,Zaiyong Jiang
Recently, the surface frustrated Lewis pairs (SFLP) have attracted more and more attention in the field of CO2 hydrogenation. The main research studies have focused on a single construction of SFLP; however, the exploration of the synergy between SFLP and other excellent techniques has been barely reported. In this work, a common photocatalyst, TiO2, was chosen as the research object and amorphous TiO2–x(OH)y and CuPt alloy were constructed on its surface to investigate the synergy between SFLP and the metal cocatalyst technique. The amorphous TiO2–x(OH)y could form effective SFLP to increase CO2 activation, and the CuPt alloy was beneficial for H2 dissociation to boost the formation of protonated/hydridic H. The synergy resulted in CuPt/TiO2–x(OH)y/TiO2 exhibiting significantly increased activity for the reverse water gas shift (RWGS) reaction compared to those of TiO2–x(OH)y/TiO2, CuPt/TiO2, and pristine TiO2. This work highlights an important research direction for the SFLP application in the field of CO2 hydrogenation.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Polymer Chemistry
·
2025
·
IF 3.9
Mei Meng,Min Xiao,Jintao Wang,Peiyuan Li,Xianli Wu,Yuezhong Meng
Carbon dioxide (CO2) has been utilized for synthesizing biodegradable polymers to promote sustainable energy conservation and mitigate emissions. Nonetheless, the low glass transition temperature of amorphous CO2-based polyester–polycarbonate (PPC-P) significantly impedes its practical application. Herein, semi-crystalline copolymers, PPC-P-co-PLA, were successfully synthesized via copolymerization of propylene oxide (PO), phthalic anhydride (PA), and CO2 in combination with PLA through transesterification catalysed by Lewis acid–base pairs in a one-pot/one-step method. Metal-free catalysts were utilized for the first time to catalyse both ring-opening copolymerization and transesterification reactions for copolymer synthesis. The mechanism study of PLA transesterification catalysed by triethyl borane (TEB)/Lewis bases revealed that effective depolymerization and transesterification of PLA hinge on α-H chemical shift alterations induced by the Lewis bases. Lewis acid–base pairs facilitate the formation of PPC-P-co-PLA multi-block copolymers by terminating one end of PPC-P with PLA segments via continuous transesterification reactions. Compared to PPC-P, the copolymers exhibit an increase in glass transition temperature by 5–7 °C and an elevation in thermal decomposition temperature by 18–45 °C. The optimal mechanical and rheological properties of PPC-P-co-PLA multi-block copolymers are achieved at a PLA concentration of 8 wt%. This study opens new avenues for the synthesis of semi-crystalline polyester–polycarbonate-based copolymers with high glass transition temperatures, thereby enriching the theoretical foundation for the synthesis of block copolymers.
研究领域:
材料科学
·
高分子化学
·
绿色化学
✓ 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）