GREEN CHEMISTRY
·
2023
·Vol. 25
·期 15
·5999-6008
·
IF 9.8
Yuanyuan Zhang,Wanxiang Zhang,Yan Wang,Shuhang Ren,Yucui Hou,Weize Wu
To reduce the emission of NO from fossil fuel combustion and the energy consumption associated with NH3 production, the development of simple and efficient methods to transform NO into high-value-added NH3 is essential. Here, we report the efficient catalytic hydrogenation of NO to NH3 under mild reaction conditions by the synergistic catalysis of functionalized ionic liquids (FILs) and Pd catalysts. In this system, an FIL [TEPA][Im] acted as both an absorbent and a catalyst. The presence of [TEPA][Im] enhanced the catalytic performance by changing the coordination and electronic environment of Pd on the Pd/C catalyst. First, NO was absorbed by [TEPA][Im]; then, the hydrogenation of absorbed NO to NH3 was performed at a low temperature via the synergistic catalyzation of [TEPA][Im] and Pd/C. The effects of various factors on NO hydrogenation to NH3 were also investigated. Remarkably, Pd/C exhibited outstanding properties in the formation of NH3 with a high yield of 67% in the FIL [TEPA][Im] under the conditions of 100 °C and an H2 pressure of 0.5 MPa. [TEPA][Im] could be reused multiple times and the product NH3 could be recovered by flashing.
研究领域:
环境化学
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催化
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Juan Du,Jiaren Zhang,Yong Sun,Wenlong Jia,Zhihao Si,He Gao,Xing Tang,Xianhai Zeng,Tingzhou Lei,Shijie Liu,Lu Lin
Catalytic transfer hydrogenation (CTH) of bio-derived furfural (FF) to furfuryl alcohol (FFA) was performed using the physically mixed CuO-Pd/C as catalyst and formic acid (FA) as hydrogen donor. The evolution investigation of Cu showed the precursor CuO firstly dissolved into Cu 2+ by FA and then formed coordination polymer-copper(II), which uniformly dispersed in reaction solution of 1, 4-dioxane. Subsequently the Cu 2+ was in-situ reduced and Cu-Pd alloys formed simultaneously. The in-situ prepared nano Cu-Pd/C catalyst exhibited the best performance with a complete FF conversion and FFA selectivity of 98.1%. Reaction conditions test suggested that the FFA selectivity was greatly dependent on the Cu content. The underlying mechanism revealed that the Pd in Cu-Pd alloys mainly promoted the FF conversion by enhancing hydrogen adsorption, while the nano Cu for increasing FFA selectivity; the Cu-Pd alloys functioned in synergistic way. Leaching and recycling tests demonstrated an excellent stability of the Cu-Pd/C catalyst.
研究领域:
化学工程
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·777-792
·
IF 2.081
Liu Yingxin,Zhang Kaiyue,Zhang Liang,Wang Yun,Wei Zuojun
The selective reductive amination of levulinic acid (LA) into pyrrolidone derivatives is regarded as one of the most promising reactions in the fields of biomass conversion into high value-added chemicals. Herein, we report a one-pot synthesis of N -substituted-5-methyl-2-pyrrolidones by reductive amination of LA/ester with nitriles over several commercial catalysts. Among the catalysts texted, Pd/C was found to be the most efficient for the reductive amination of LA/ester with various nitriles to give high yields of pyrrolidones (up to 92%) under mild reaction conditions (80 °C, 1.6 MPa H 2 , tetrahydrofuran solvent). And the catalyst showed good reusability.
研究领域:
化学工程
·
有机化学
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生物质转化
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yong Xu,Yue Wang,Ping Wang,Yishun Wang,Weili Dai,Jianping Zou,Xubiao Luo
Employing electric energy to convert carbon dioxide (CO 2 ) into valuable small molecules is a potentially practical method in energy storage and greenhouse gas alleviation. A huge challenge for electrocatalytic CO 2 reduction is to reduce overpotential to improve energy efficiency. Herein, we demonstrate that doping alloy Pd 49 Ag 30 Te 4 (PAT) with rare-earth element Tb is beneficial for selective exposure of (1 1 1) crystal plane, which is a highly active crystal plane for producing carbon monoxide (CO). The as-prepared Tb 2.9 PAT exhibited high electrocatalytic performance with 95.7 % CO faradic efficiency at − 0.8 V (vs RHE), far exceeding that of PAT, and coupled with good durability. In situ spectral study and theoretical calculations disclose that the introduction of Tb regulates the d-band center of PAT alloy, weakens the Pd − C bonding ability, and promotes the desorption of *CO in the rate-determining step. This study provides a method for doping induced selective exposure of crystal face, which provides new idea for improving catalytic performance.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Riyang Shu,Ying Xu,Longlong Ma,Qi Zhang,Chao Wang,Ying Chen
Many effective methods have been proposed to achieve lignin depolymerization, while controllable product distribution is still hard to realize. Herein, an efficient lignin hydrogenolysis process with controllable product distribution was put forward using Pd/C catalyst cooperated with metal chloride. Results showed that lignin produced a high amount of guaiacols in the presence of ZnCl 2 , while a high amount of phenols in the presence of CrCl 3 . Guaiacylglycerol-β-guaiacyl ether was used as the model compound to carry out the mechanistic investigation. A synergetic catalysis effect between Pd/C and metal chloride was exhibited in this process. And the Lewis acidity was an important factor to determine the product distribution. With the synergetic catalysis of Pd/C and metal chloride, the dissociation energy of β-O-4 bond was reduced significantly, which made the cleavage easier to realize. The phenolic monomer product of guaiacols was produced in the initial stage. Then CrCl 3 catalyst with strong Lewis acidity could further promote the occurrence of demethoxylation and alkylation, converting the guaiacols into phenols. This work figures out the mechanism of product control in the hydrogenolysis process and displays a clear potential for the controllable valorization of lignin.
研究领域:
化学工程
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催化
·
可再生能源
·
有机化学
✓ 已验证
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Dongxuan He,Gang Wang,Binghan Li,Junrong Huang,Shuming Dou,Wei Gan,Hengzhi You,Qunhui Yuan
Tris(hydroxymethyl)aminomethane (Tris) and its derivatives serve as crucial biological buffers. Presently, Tris is predominantly synthesized by reducing tris(hydroxymethyl)nitromethane using conventional reducing agents such as hydrazine hydrate and metal powders. However, hydrazine hydrate poses a significant threat to aquatic life, while the use of reducing metal powders generates substantial solid waste, thereby exerting considerable environmental pressure in terms of green and sustainable chemistry. The utilization of non-homogeneous catalysts for hydrogenation reduction offers a viable solution to mitigate these issues. Yet, the exploration of non-homogeneous catalysts remains incomplete and lacks comprehensive research. In this study, a highly active Pd/C catalyst for the hydrogenation reduction of tris(hydroxymethyl)nitromethane was fabricated, through an ultrarapid high-temperature thermal shock (HTS) synthesis. The ultrafine Pd particles (∼5.5 nm) are uniformly distributed on the carbon substrate, rendering the catalyst high activity and stability. Additionally, we successfully combine this heterogeneous catalyst with continuous flow technology and achieve a continuous and stable production of Tris for more than 8 h, with a satisfying yield of ∼96%. This report may shed light on the efficient fabrication of more ultrafine catalysts for hydrogenation reductions with high noble-metal utilization.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 9
·2889-2900
·
IF 9.48
Song Li,Long Yan,Qiying Liu,Jianguo Liu,Qiyu Liu,Wei Fan,Xuelai Zhao,Xinghua Zhang,Chenguang Wang,Longlong Ma,Qi Zhang
One-pot hydrodeoxygenation (HDO) of biomass furan derivatives into long-chain alkanes remains unclear owing to the complicated reactions at high temperatures. Here, Pd/C combined with phosphotungstic acid (HPW), a strong Brønsted solid acid promoter, was developed to produce decane under mild conditions through the one-pot HDO of δ-furfurylidenelevulinic acid (FDLA). A 93.16% sum yield of alkanes including 89.53% yield of decane was obtained under 3 MPa H2 at 170 °C for 4 h. The ring-opening and HDO of furans are accomplished at preheating stage, which enable to clarify the complicated reaction pathway. In addition, experimental validations and catalytic characterizations confirm that the synergistic effect of active acid–metal sites plays a critical role in the generation of alkanes via the formation and hydrogenolysis of lactone intermediates to aldehyde/alcohol. This work provides guidance for the one-pot HDO of biomass furan derivatives via the combination of metal catalyst and strong Brønsted solid acid under mild conditions.
研究领域:
化学工程
·
催化
·
可再生能源
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Mengyu Dou,Yan Qiao,Xu Hu,Hengyang Miao,Ligong Zhou,Xuekuan Li,Xianglin Hou,Yingxiong Wang,Mingxing Tang
The poor textural properties of initial biochar materials have hindered their extensively applied as catalyst supports. Herein, cellulose biochar materials with the gradient porous and high specific surface area were synthesized by adding different ratios of ZnCl 2 , and as supports to prepare Pd/C cel catalysts for efficient maleic acid hydrogenation in water. The characterization results indicated that the textural propertiesand dispersion of Pd in Pd/C cel catalysts depended on the ratio of ZnCl 2 to cellulose. The Pd/C cel ZnCl 2(1:3) catalyst exhibited the best catalytic activity among all catalysts and outstanding stability for reusing 8 times under mild conditions (60 °C, 2 MPa). In addition, this synthesis strategy was also suitable for other biomass materials (glucose, sucrose, and starch) and the catalytic performance of ZnCl 2 -modified Pd/C catalysts in maleic acid hydrogenation reaction also improved dramatically. The carbonization mechanism was discussed by TG-MS and the results illustrated that ZnCl 2 reduced the carbonization temperature and altered the pyrolysis behavior of biochar as a result of excellent catalytic behavior. This work provided a facile and universal strategy for synthesizing biochar high-efficient supported catalysts with gradient porous structure and high specific surface area.
研究领域:
催化
·
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2021
·
IF 5.565
Weilai Wang,Fan Zhang,Yunfei Zhang,Lei Xu,Yuansheng Pei,Junfeng Niu
Hydrodechlorination is a promising technology for the remediation of water body contaminated with trichloroethylene (TCE). In this work, the liquid-phase hydrogenation of TCE by Raney Ni (R-Ni) and Pd/C under an open system have been studied, in which nascent H 2 (Nas-H 2 ) generated in situ from the cathode acted as a hydrogen source. Experimental results showed that TCE was completely eliminate from the solution through the synergistic effects of hydrodechlorination and air flotation due to the formation of continuous micro/nano-sized Nas-H 2 bubbles from the cathode. Furthermore, the effects of inorganic anions and organic solvents on R-Ni and Pd/C hydrogenation activity were investigated, respectively. The results showed that NO 3 − and acetonitrile can form a competitive reaction with TCE; Sulfur with lone-pair electrons will cause irreversible poisoning to these two catalysts, and have a stronger inhibitory effect on Pd/C. This work helps to realize the separation of volatile halogenated compounds from water environment and provides certain data support for the choice of catalyst in the actual liquid-phase hydrogenation system.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2023
·
IF 4.1
Ning Shi,Tianlang Zhu,Hongyan Zhang,Hongsheng Huang,Liang Zhou,Ying Liu,Riyang Shu
Catalytic conversion of cellulose into the novel platform molecule 2,5-hexanedione (HXD) is regarded as one feasible approach for high-value utilization of biomass resources. Here, we reported one efficient way of one-pot conversion of cellulose into HXD with high yield of 80.3% in H2O and tetrahydrofuran (THF) mixture within Al2(SO4)3 combined with Pd/C as a catalyst. In the catalytic reaction system, Al2(SO4)3 could catalyze the conversion of cellulose into 5-hydroxymethylfurfural (HMF), and Pd/C combined with Al2(SO4)3 could catalyze the hydrogenolysis of HMF into furanic intermediates such as 5-methylfurfuryl alcohol and 2,5-dimethylfuran (DMF) without causing over-hydrogenation of these furanic intermediates. These furanic intermediates were finally transformed into HXD catalyzed by Al2(SO4)3. Besides, the H2O/THF ratio could significantly influence the reactivity of the hydrolytic furanic ring-opening of the furanic intermediates. The catalytic system also showed excellent performance on the conversion of other carbohydrates (glucose and sucrose) into HXD.
研究领域:
生物质化学
·
催化反应工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Asia-Pacific Journal of Chemical Engineering
·
2024
·
IF 1.4
Bo Wang,Pei-ya Li,Shu-han Lu,Bin Wang,Fusheng Yang,Tao Fang
Liquid organic hydrogen carrier (LOHC) technology has unique advantages in hydrogen storage and transportation. However, the lack of research on the continuous dehydrogenation process of LOHCs has hindered the design and application of industrial dehydrogenation processes. In this work, a highly active dehydrogenation catalyst 1.5 wt% Pd/activated carbon (Pd/C) and a commercial catalyst 5 wt% Pd/Al 2 O 3 were used for the continuous dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC). Based on a tubular reactor and lab-scale apparatus, 1.5 wt% Pd/C catalyst achieved a maximum dehydrogenation conversion of 98.3% and a maximum NEC selectivity of 95.3%, while dehydrogenation conversion and NEC selectivity with 5 wt% Pd/Al 2 O 3 were 98.3% and 97.6%, respectively. It showed the equally excellent performance between Pd/C and Pd/Al 2 O 3 , and the former has less Pd loading than the latter, with the potential of reducing the production cost of the dehydrogenation catalyst. The dehydrogenation results also indicated the difference in catalytic performance between the two kinds of catalysts. The obtained kinetics data were analyzed, and the dynamics of continuous dehydrogenation were studied to provide fundamental information for dehydrogenation scale-up.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 151
·期 10
·3004-3010
·
IF 3.186
Zhou Junjie,Huang Yu,Shen Jialu,Liu Xiang
The production of H 2 from non-fossil sources is a key research challenge to contributing solving the forthcoming energy problem. Aqueous solutions of tetrahydroxydiboron have very recently appeared as a H 2 source, from which both hydrogen atoms are provided by water, in the presence of highly sophisticated nanocatalysts. Herein, commercial and cheap Pd/C is shown to be an efficient and recyclable catalyst for H 2 evolution upon tetrahydroxydiboron hydrolysis. Graphic Abstract
研究领域:
化学
·
能源科学
✓ 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）