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Catalysts · 2020 ·Vol. 10 ·期 9 ·1027 · IF 3.52

Solution Combustion Synthesis of Fe2O3-Based Catalyst for Ammonia Synthesis

Binxiang Cai,Huazhang Liu,Wenfeng Han

Fe2O3-based catalysts were prepared by solution combustion synthesis (SCS) with metal nitrates (Fe, K, Al, Ca) as the precursors and glycine as the fuel. The activities of catalysts were evaluated in terms of ammonia synthesis reaction rate in a fixed bed reactor similar to the industrial reactors. The results indicate that the precursor of catalyst prepared by SCS is Fe2O3which facilitates the high dispersion of promoters to provide high activity. The catalysts exhibit higher activity for ammonia synthesis than that of traditional catalysts, and the reaction rate reaches 138.5 mmol g−1h−1. Fe2O3prepared by SCS could be favorable precursor for ammonia synthesis catalyst. The present study provides a pathway to prepare catalyst for ammonia synthesis.Keywords:ammonia synthesis;catalyst;Fe2O3;solution combustion synthesis

研究领域: 化学工程 · 催化科学
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NATURE BIOTECHNOLOGY · 2025 · IF 41.7

Scaling DNA synthesis with a microchip-based massively parallel synthesis system

Zhang Xiandi,Jiang Xiang’er,Wang Yun,Chen Qinzhen,Jiang Hao,Zhang Hu,Beltran Antoni,Yang Weiya,Chen Tai,Liang Chenglong,Cheng Ning,Huang Yun,Ding Guqiao,Xie Chengwang,Gao Nanfeng,Liu Juntao,Xu Wei,Huang Jinlei,Cai Dong,Zhu Lihao,Mo Songjin,Shen Mengzhe,Zhang Wenwei,Lehner Ben,Ni Ming,Wang Jian,Xu Xun,Shen Yue

Current high-throughput DNA synthesis technologies use intricate chip and microfluidic systems to produce large-scale synthetic oligonucleotides but with low concentration and limited compatibility for long DNA assembly. Here we report a massive-in-parallel synthesis system, with an ‘identification–sorting–synthesis–recycling’ iteration mechanism applied to microchips for high-throughput DNA synthesis. This approach increases DNA product concentration by four to six orders of magnitude and simplifies downstream processes for large-scale gene synthesis.

CAS / MDL: 148893-10-1 7087-68-5
研究领域: 分子生物学 · 合成生物学 · 生物技术 · 基因工程 · 高通量筛选
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Catalysis Science & Technology · 2019 ·Vol. 9 ·期 13 ·3454-3468 · IF 5.726

Nanoparticles of Rh confined and tailored by LaFeO3–La2O3 on SiO2 for direct ethanol synthesis from syngas

Huixian Zhong,Jiaming Wang,Kang An,Kegong Fang,Yuan Liu

A catalyst with a novel composition for direct ethanol synthesis from syngas was prepared and investigated in this work, which is Rh nanoparticles (NPs) highly dispersed on La2O3 modified LaFeO3, and the Rh NPs/La2O3–LaFeO3 was loaded on SiO2 with high surface area. The catalyst was prepared by using LaFe1−xRhxO3 in the perovskite phase as the precursor, which was transformed to Rh/La2O3–LaFeO3/SiO2 after reduction. The results showed that, compared to Rh–La2O3/SiO2, the activity and selectivity to ethanol were improved markedly, which was ascribed to the well-matched catalyzing process by the active sites of Rh0, Rh+ (or Rhδ+) and the oxygen vacancies on the surface of LaFeO3; of those, Rh0 dissociatively adsorbed CO and the latter two associatively adsorbed CO. Moreover, the interaction of La2O3 and LaFeO3 donated electrons to rhodium, which effectively adjusted the ratio of CO adsorbed associatively and dissociatively, and thus improved the selectivity to ethanol and lowered the selectivity to methanol. The catalyst also exhibited excellent resistance to the sintering of Rh NPs and to carbon deposition, which was attributed to the confinement of Rh NPs by La2O3 and LaFeO3, the eliminating effect of La2O3 and LaFeO3 and the very high dispersion of Rh NPs.

研究领域: 催化化学 · 材料科学
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Scientific Reports · 2016 ·Vol. 6 ·期 1 ·1-8 · IF 5.228

Functional characterization of ent-copalyl diphosphate synthase, kaurene synthase and kaurene oxidase in the Salvia miltiorrhiza gibberellin biosynthetic pathway

Su Ping,Tong Yuru,Cheng Qiqing,Hu Yating,Zhang Meng,Yang Jian,Teng Zhongqiu,Gao Wei,Huang Luqi

Salvia miltiorrhiza Bunge is highly valued in traditional Chinese medicine for its roots and rhizomes. Its bioactive diterpenoid tanshinones have been reported to have many pharmaceutical activities, including antibacterial, anti-inflammatory and anticancer properties. Previous studies found four different diterpenoid biosynthetic pathways from the universal diterpenoid precursor ( E , E , E )-geranylgeranyl diphosphate (GGPP) in S. miltiorrhiza . Here, we describe the functional characterization of ent -copalyl diphosphate synthase (SmCPS ent ), kaurene synthase (SmKS) and kaurene oxidase (SmKO) in the gibberellin (GA) biosynthetic pathway. SmCPS ent catalyzes the cyclization of GGPP to ent -copalyl diphosphate ( ent -CPP), which is converted to ent -kaurene by SmKS. Then, SmKO catalyzes the three-step oxidation of ent -kaurene to ent -kaurenoic acid. Our results show that the fused enzyme SmKS-SmCPS ent increases ent -kaurene production by several fold compared with separate expression of SmCPS ent and SmKS in yeast strains. In this study, we clarify the GA biosynthetic pathway from GGPP to ent -kaurenoic acid and provide a foundation for further characterization of the subsequent enzymes involved in this pathway. These insights may allow for better growth and the improved accumulation of bioactive tanshinones in S. miltiorrhiza through the regulation of the expression of these genes during developmental processes.

CAS / MDL: 18107-18-1
研究领域: 植物学 · 药用植物研究 · 分子生物学
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Catalysts · 2018 ·Vol. 8 ·期 6 ·249 · IF 3.465

Enzymatic Synthesis of Thioesters from Thiols and Vinyl Esters in a Continuous-Flow Microreactor

Nani Zhou,Le Shen,Zhen Dong,Jiahong Shen,Lihua Du,Xiping Luo

The preparation of thioesters through the lipase-catalysed transesterification reaction of thiols with vinyl carboxyl esters is described. The reactions were carried out by Lipase TL IM fromThermomyces lanuginosusas a catalyst and performed under a continuous flow microreactor. We first found that lipase TL IM can be used in the reaction of thioester synthesis with high efficiency. Various reaction parameters were investigated including substrate molar ratio, reaction time, and temperature. Maximum conversion (96%) was obtained under the optimal condition of a substrate molar ratio of 1:2 (4-methylbenzyl mercaptan:vinyl esters) at 50 °C for about 30 min. Compared with other methods, the salient features of this work include mild reaction conditions (50 °C), short reaction times (30 min), high yields, and environment-friendliness.Keywords:enzymatic synthesis;thioester synthesis;flow chemistry;microreactor

研究领域: 生物化学 · 有机化学
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Chem · 2024 · IF 19.1

Selective nitrogen fixation via Janus C-N coupling in co-electrolysis

Xiaoran Zhang,Xiaorong Zhu,Shuowen Bo,Chen Chen,Qingfeng Zhai,Shuang Li,Xiaojin Tu,Jianyun Zheng,Dongdong Wang,Xiaoxiao Wei,Wei Chen,Tehua Wang,Yafei Li,Qinghua Liu,San Ping Jiang,Liming Dai,Shuangyin Wang

Electrocatalysis offers a sustainable approach to artificial nitrogen fixation yet faces numerous challenges. Selective synthesis of nitrogen-containing compounds shows promise but needs significant improvement. Herein, we demonstrate selective ammonia and urea synthesis via co-electrolysis with CO 2 . High CO binding energy on Re-Mn catalysts leads to the formation of ∗C species, which serve as electron reservoirs to enhance N 2 activation for C-N coupling (N 2  + ∗C → ∗CN 2 ), followed by C-N dissociation. This results in ammonia production with a yield rate of 48.9 ± 2.4 mg g −1 h −1 and an N-selectivity of 98.4%. In contrast, Zn-Mn sites, characterized by low CO binding, facilitate the migration of CO and its coupling with adsorbed N 2 (CO + ∗N=N∗ → ∗NCON∗). Subsequent hydrogenations of ∗NCON∗ promote urea synthesis with an N-selectivity of 89.1%. Utilizing Janus coupling with two C-N pathways aims to meet energy, agriculture, and chemical industry demands. We realized the selective synthesis of ammonia and urea, respectively, in one electrocatalytic system for the first time by Janus coupling with two distinguishable C-N coupling paths from N 2 and CO 2 .

研究领域: 化学工程 · 能源科学 · 农业科学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

In situ topochemical carbonization derivative Co-Ni alloy@Co-Co2C for direct ethanol synthesis from syngas

Jiaming Wang,Guilong Liu,Huixian Zhong,Pengfei Song,Kang An,Ziyang Zhang,Ang Cao,Yuan Liu

In this work, Co δ+ -Co 2 C decorated-Co-Ni alloy nanoparticles (NPs) loaded on Mg-Al-O complex oxides were fabricated via an in-situ reduction and topochemical carbonization strategy by using hydrotalcite as the precursor. The Co δ+ -Co 2 C decorated-Co-Ni alloys were obtained via the following process: (I) after reduction, Co-Ni alloy was obtained and Co could donate electrons to Ni in the Co-Ni alloy NPs; (II) in syngas atmosphere, some of cobalt atoms on the surface of Co-Ni NPs reacted with CO and were converted to Co 2 C. Resultantly, in the reaction process, Co-Ni alloy NPs were transformed into Ni-Co alloy@Co-Co 2 C, a core-shell structure with Ni-Co alloy core and Co-Co 2 C shell. When used as the catalysts for direct ethanol synthesis (DES) from syngas, the bimetallic Co-Ni alloy@Co-Co 2 C catalyst performed excellent selectivity to ethanol, owing to the regulation of dissociatively and associatively adsorbed CO by Co δ+ -Co 2 C active sites formed on the surface of Co-Ni alloy NPs. Moreover, the mutual dilution between Co and Ni in the Co-Ni alloy NPs inhibited the generation of heavy hydrocarbons, further improving the selectivity to alcohols. The total alcohol selectivity of 43.0% and ethanol occupied 45.2 wt% could be reached over the optimal catalyst.

研究领域: 材料科学 · 催化化学
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JOURNAL OF CHEMICAL RESEARCH · 2015 · IF 0.633

A Novel and Efficient Synthesis of Anti-Cancer Agent, Mereletinib

Haidong Liu,Yongfeng Lv,Yuan Li,Jin Cai,Junqing Chen,Yu Qin,Min Ji

A convenient route for the synthesis of a third-generation epidermal growth factor receptor inhibitor, mereletinib (AZD9291) using starting materials that are commercially available has been achieved through reactions that are readily conducted under mild conditions. Importantly, a 5 g scale synthesis was also accomplished and this method could therefore be useful in the synthesis of similar drugs.

研究领域: 药物化学 · 有机合成 · 肿瘤学
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Frontiers of Chemical Science and Engineering · 2024 ·Vol. 18 ·期 10 ·1-10 · IF 4.3

Conversion of syngas into lower olefins over a hybrid catalyst system

Zhao Qiao,Wang Hongyu,Liang Haoting,Han Xiaoxue,Wei Chongyang,Wang Shiwei,Wang Yue,Huang Shouying,Ma Xinbin

Lower olefins, produced from syngas through Fischer-Tropsch synthesis, has been gaining worldwide attention as a non-petroleum route. However, the process demonstrates limited selectivity for target products. Herein, a hybrid catalyst system utilizing Fe-based catalyst and SAPO-34 was shown to enhance the selectivity toward lower olefins. A comprehensive study was conducted to examine the impact of various operating conditions on catalytic performance, such as space velocity, pressure, and temperature, as well as catalyst combinations, including loading pattern, and mass ratio of metal and zeolite. The findings indicated that the addition of SAPO-34 was beneficial for enhancing catalytic activity. Furthermore, compared with AlPO-34 zeolite, the strong-acid site on SAPO-34 was identified to crack the long-chain hydrocarbons, thus contributing to the lower olefin formation. Nevertheless, an excess of strong-acid sites was found to detrimentally impact the selectivity of lower olefins, attributed to the increased aromatization and polymerization of lower olefins. The detailed analysis of a hybrid catalyst in Fischer-Tropsch synthesis provides a practical strategy for improving lower olefins selectivity, and has broader implications for the application of hybrid catalyst in diverse catalytic systems.

研究领域: 化学工程 · 催化科学
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Jove-Journal of Visualized Experiments · 2019 · IF 1.108

Biosynthesis of a Flavonol from a Flavanone by Establishing a One-pot Bienzymatic Cascade

Zhiping Zhang,Shuhang Fan,Zhiqiang Chen,Yanzhi He,Mengfei Huang,Li Ding,Yanyan Zhang,Lin Chen,Xinyue Zhang

Flavonols are a major subclass of flavonoids with a variety of biological and pharmacological activities. Here, we provide a method for the in vitro enzymatic synthesis of a flavonol. In this method, Atf3h and Atfls1, two key genes in the biosynthetic pathway of the flavonols, are cloned and overexpressed in Escherichia coli. The recombinant enzymes are purified via an affinity column and then a bienzymatic cascade is established in a specific synthetic buffer. Two flavonols are synthesized in this system as examples and determined by TLC and HPLC/LC/MS analyses. The method displays obvious advantages in the derivation of flavonols over other approaches. It is time- and labor-saving and highly cost-effective. The reaction is easy to be accurately controlled and thus scaled up for mass production. The target product can be purified easily due to the simple components in the system. However, this system is usually restricted to the production of a flavonol from a flavanone.

CAS / MDL: 117-39-5
研究领域: 生物化学 · 分子生物学
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TETRAHEDRON · 2022 · IF 2.388

A fungal nonribosomal peptide-polyketide hybrid synthase synthesizes 2-pyrrolidinone alkaloid

Li Rao,Hu-Cheng Shi,Yi Zou

A new fungal nonribosomal peptide-polyketide hybrid synthase , namely CogA, was discovered by genome mining from fungus Cordyceps gunnii . Its ability to synthesize 4-hydroxyl 2-pyrrolidinone alkaloid ( 1 ) via nonenzyme-catalyzed N-1-C-2 closure was confirmed by heterologous expression of it in Aspergillus nidulans . Further engineered biosynthesis of the fluoro-substituted 2-pyrrolidinone alkaloid analogues ( 4 and 5 ) has also been achieved in vivo .

研究领域: 真菌学 · 合成生物学 · 生物化学
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2019 · IF 3.571

Significantly Enhanced Production of Patchoulol in Metabolically Engineered Saccharomyces cerevisiae

Bin Ma,Min Liu,Zhen-Hai Li,Xinyi Tao,Dong-Zhi Wei,Feng-Qing Wang

Patchoulol, a natural sesquiterpene compound, is widely used in perfumes and cosmetics. Several strategies were adopted to enhance patchoulol production in Saccharomyces cerevisiae: (i) farnesyl pyrophosphate (FPP) synthase and patchoulol synthase were fused to increase the utilization of FPP precursor; (ii) expression of the limiting genes of the mevalonate pathway was enhanced; (iii) squalene synthase was weakened by a glucose-inducible promoter of HXT1 (promoter for hexose transporter) to reduce metabolic flux from FPP to ergosterol; and (iv) farnesol biosynthesis was inhibited to decrease the consumption of FPP. Glucose was used to balance the trade-off between the competitive squalene and patchoulol pathways. The patchoulol production was 59.2 ± 0.7 mg/L in a shaken flask with a final production of 466.8 ± 12.3 mg/L (20.5 ± 0.5 mg/g dry cell weight) combined with fermentation optimization, which was 7.8-fold higher than the reported maximum production. The work significantly promoted the industrialization process of patchoulol production using biobased microbial platforms.

CAS / MDL: 4602-84-0 5986-55-0
研究领域: 生物技术 · 代谢工程 · 生物过程工程
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