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formic acid Dehydrogenation for Hydrogen Production Promoted by Grubbs and Hoveyda-Grubbs Catalysts

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Chinese Journal of Chemistry 2021年第8期39卷 2201-2206页

作者： Qian Wang Yihao Xia Fanrui Cheng Zhijian Chen Yifan Wang Xiaofei Zhu Lei Qin Zhiping Zheng School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbinHeilongjiang 150001China Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055China School of Chemistry and Life Science Changchun University of TechnologyChangchunJilin 130012China Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhenGuangdong 518055China

In this work,we screened three Grubbs catalysts and two Hoveyda-Grubbs catalysts for the production of H_(2) by dehydrogenation of formic acid(FA).The best results were achieved with the use of a first-generation Hoveyda-Grubbs *** a catalyst loading of mere 0.5μmol, a maximum TON of 36356 was obtained within 3 *** key intermediates were identified by using 1H NMR and high-resolution electrospray ionization mass spectroscopy(HRESI-MS),based on which a mechanism possibly responsible for the observed catalysis was proposed.

关键词： Hydrogen formic acid Grubbs and Hoveyda-Grubbs catalysts Ruthenium Dehydrogenation

Amine-functionalized hierarchically porous carbon supported Pd nanocatalysts for highly efficient H2 generation from formic acid with fast-diffusion channels

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Journal of Energy Chemistry 2023年第1期76卷 249-258,I0007页

作者： Xianzhao Shao Xinyi Miao Fengwu Tian Miaomiao Bai Xiaosha Guo Wei Wang Zuoping Zhao Xiaohui Ji Miyi Li Fangan Deng Shaanxi Key Laboratory of Catalysis School of Chemistry and Environment ScienceShanxi University of TechnologyHanzhong 723001ShaanxiChina School of Mathematics and Computer Science Shanxi University of TechnologyHanzhong 723001ShaanxiChina State Key Laboratory of Qinba Bio-Resource and Ecological Environment Shaanxi University of TechnologyHanzhong 723001ShaanxiChina School of Chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 102488China

formic acid(FA)has come to be considered a potential candidate for hydrogen storage,and the development of efficient catalysts for H2releasing is crucial for realizing the sustainable process from ***,we have developed the ultrafine Pd nanoparticle(NPs)with amine-functionalized carbon as a support,which was found to show an excellent catalytic activity in H_(2)generation from FA *** synergetic mechanism between amine-group and Pd active site was demonstrated to facilitate H2generation byβ-hydride ***,the texture of support for Pd NPs also plays an important role in determining the reactivity of FA,since the diffusion of gaseous products makes the kinetics of diffusion as a challenge in this high performance Pd *** a result,the as-prepared Pd/NH_(2)-TPC catalyst with the small sized Pd nanoparticles and the hierarchically porous structures shows a turnover of frequency(TOF)value of 4312 h^(-1)for the additive-free FA dehydrogenation at room temperature,which is comparable to the most promising heterogeneous *** results demonstrated that the intrinsic catalytic activities of active site as well as the porous structure of support are both important factors in determining catalytic performances in H2generation from FA dehydrogenation,which is also helpful to develop high-activity catalysts for other advanced gas-liquid-solid reactions systems.

关键词： Hierarchically carbon Diffusion formic acid Hydrogen production Palladium nanoparticles

Synthesis of palladium-rhodium bimetallic nanoparticles for formic acid dehydrogenation

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Journal of Energy Chemistry 2021年第1期30卷 301-309,I0010页

作者： Ilaria Barlocco Sofia Capelli Elisa Zanella Xiaowei Chen Juan JDelgado Alberto Roldan Nikolaos Dimitratos Alberto Villa Dipartimento di Chimica Universitàdegli Studi di MilanoMilan I-20133Italy Departamento de Ciencia de los Materiales Ingeniería Metalúrgica y Química InorgánicaFacultad de CienciasUniversidad de CádizCampus Río San PedroPuerto Real(Cádiz)E-11510Spain School of Chemistry Cardiff UniversityMain BuildingPark PlaceCF103AT CardiffUnited Kingdom Dipartimento di Chimica Industriale e dei Materiali Alma Mater Studiorum Universitàdi BolognaViale Risorgimento 4I-40136 BolognaItaly

Herein,we report for the first time the synthesis of preformed bimetallic Pd-Rh nanoparticles with different Pd:Rh ratios(nominal molar ratio:80-20,60-40,40-60,20-80) and the corresponding Pd and Rh monometallic ones by sol immobilization using polyvinyl alcohol(PVA) as protecting agent and NaBH4 as reducing agent,using carbon nanofibers with high graphitization degree(HHT) as the desired *** synthesized catalysts were characterized by means of Transmission Electron Microscopy(TEM) and inductively coupled plasma optical emission spectroscopy(ICP-OES).TEM shows that the average particle size of the Pd-Rh nanoparticles is the range of 3-4 nm,with the presence of few large agglomerated *** bimetallic catalysts,EDX-STEM analysis of individual nanoparticles demonstrated the presence of random-alloyed nanoparticles even in all cases Rh content is lower than the nominal one(calculated Pd:Rh molar ratio:90-10,69-31,49-51,40-60).The catalytic performance of the Pd-Rh catalysts was evaluated in the liquid phase dehydrogenation of formic acid to *** was found that Pd-Rh molar ratio strongly influences the catalytic ***-rich catalysts were more active than Rh-rich ones,with the highest activity observed for Pd90:Rh10(1792 h^(-1)),whereas Pd69:Rh31(921 h^(-1)) resulted the most stable during recycling ***,Pd90:Rh10 was chosen as a representative sample for the liquid-phase hydrogenation of muconic acid using formic acid as hydrogen donor,showing good yield to adipic acid.

关键词： Palladium Rhodium Alloy formic acid Hydrogen Muconic acid

One-step synthesis of Ni@Pd/NH_(2)-Fe_(3)O_(4)nanoparticles as affordable catalyst for formic acid dehydrogenation

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Chinese Journal of Chemical Engineering 2021年第4期34卷 168-174页

作者： Mohammad Reza Nabid Yasamin Bide Mahsa Jafari Department of Polymer&Material Chemistry Faculty of Chemistry&Petroleum ScienceShahid Beheshti UniversityTehran ***Iran

Currently,one of the critical issues in the world is finding an appropriate green alternative to fossil fuels due to the concerns about global *** a hydrogen source,formic acid has been given particular attention owing to the attractive features such as highenergy density,no toxicity,high stability at ambient temperature and high hydrogen *** an affordable and highly efficient catalyst with easy recovery from the reaction mixture for selective dehydrogenation of formic acid is still *** this report,we used a simple onestep process to synthesize Ni@Pd core shell nanoparticles on 3aminopropyltriethoxysilane modified Fe3O4 *** existence of Ni and Pd results in a synergic effect on the catalytic ***—NH2 groups play an important role for obtaining welldispersed ultrafine particles with high surface area and active *** addition,Fe3O4 lead to convenient magnetic recovery of the catalyst from reaction *** results indicate that the asprepared catalyst give the superb turnover frequency of 5367.8 h 1 with no additive,which is higher than most of the previously reported catalysts.

关键词： Core-shell Fe_(3)O_(4) Catalysis Dehydrogenation formic acid

Enhanced reductive degradation of carbon tetrachloride by carbon dioxide radical anion-based sodium percarbonate/ Fe（ll）/formic acid system in aqueous solution

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Frontiers of Environmental Science & Engineering 2018年第2期12卷 61-70页

作者： Wenchao Jiang Ping Tang Shuguang Lu Xiang Zhang Zhaofu Qiu Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and Technology Shanghai 200237 China

The performance of sodium percarbonate （SPC） activated with ferrous ion （Fe（Ⅱ） with the addition of formic acid （FA） to stimulate the degradation of carbon tetrachloride （CT） was investigated. Results showed that CT could be entirely reduced within 15 min in the system at a variety of SPC/Fe（Ⅱ）/FA/CT molar ratios in experimental level. Scavenging tests indicated that carbon dioxide radical anion （CO2-） was the dominant reactive oxygen species responsible for CT degradation. CT degradation rate, to a large extent, increased with increasing dosages of chemical agents and the optimal molar ratio of SPC/Fe（Ⅱ）/FAJCT was set as 60/60/60/1. The initial concentration of CT can hardly affect the CT removal, while CT degradation was favorable in the pH range of 3.0-9.0, but apparently inhibited at pH 12. C1- and HCO3 of high concentration showed negative impact on CT removal. Cl- released from CT was detected and the results confirmed nearly complete mineralization ofCT. CT degradation was proposed by reductive C-C1 bond splitting. This study demonstrated that SPC activated with Fe（Ⅱ） with the addition of FA may be promising technique for CT remediation in contaminated groundwater.

关键词： Carbon tetrachloride Sodium percarbonate formic acid Reductive radicals Groundwater

FeOx Coating on Pd/C Catalyst by Atomic Layer Deposition Enhances the Catalytic Activity in Dehydrogenation of formic acid

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Chinese Journal of Chemical Physics 2017年第3期30卷 319-324,I0002页

作者：李俊杰路军岭中国科学技术大学化学物理系合肥微尺度国家科学实验室能源材料化学协同创新中心中国科学院能量转换材料重点实验室合肥230026

Hydrogen generation from formic acid （FA） has received significant attention. The challenge is to obtain a highly active catalyst under mild conditions for practical applications. Here atomic layer deposition （ALD） of FeOx was performed to deposit an ultrathin oxide coating layer to a Pd/C catalyst, therein the FeOx coverage was precisely controlled by ALD cycles. Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of Pd nanoparticles （NPs）. X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the Pd NPs caused a positive shift of Pd3d binding energy. In the FA dehydrogenation reaction, the ultrathin FeOx layer on the Pd/C could considerably improve the catalytic activity, and Pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one. shape as a function of the number of FeOx ALD The improved activities were in a volcanocycles, indicating the coverage of FeOx is critical for the optimized activity. In summary, simultaneous improvements of activity and thermal stability of Pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction.

关键词： formic acid Hydrogen generation Atomic layer deposition FeOx coating Pd catalyst

Electrochemical reduction of carbon dioxide to produce formic acid coupled with oxidative conversion of biomass

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Journal of Energy Chemistry 2024年第5期92卷 705-729页

作者： Xi Liu Yifan Wang Zhiwei Dai Daihong Gao Xuebing Zhao Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Institute of Applied Chemistry Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon *** is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical *** is the most abundant renewable resource in the natural *** biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon *** this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added ***-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction ***-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis *** was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.

关键词： Electrochemical reduction of CO_(2) formic acid Oxidative conversion of biomass Lignocellulose Coupled system

Enhanced formic acid production for CO₂ photocatalytic reduction over Pd/H-TiO₂ catalyst

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FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING 2024年第11期18卷 134-134页

作者： Gao, Huimin Zhang, Jinpeng Zhang, Fangyuan Jing, Jieying Li, Wen-Ying Taiyuan Univ Technol State Key Lab Clean & Efficient Coal Utilizat Taiyuan 030024 Peoples R China Shanxi Zheda Inst Adv Mat & Chem Engn Taiyuan 030000 Shanxi Peoples R China

The photocatalytic reduction of CO2 into formic acid is a feasible approach to alleviate the effects of global climate change and achieve chemical energy storage. It is important to design highly active photocatalysts to improve the selectivity and yield of formic acid. In this study, TiO2-based catalysts were prepared and loaded with Pd nanoparticles via an impregnation process. The Pd/H-TiO2 catalyst demonstrated superior CO2 reduction activity and a high formic acid production rate of 14.14 mmol(cat)g(-1)h(-1). The excellent catalytic performance observed in the presence of a Pd/H-TiO2 catalyst is ascribed to the synergy between O-v and Pd. The presence of O-v led to increase in CO2 adsorption while Pd loading enhanced the photogenerated electron-hole pair separation. Electron transfer from H-TiO2 to Pd also contributed to CO2 activation.

关键词： CO2 reduction formic acid photocatalysis TiO2 catalyst

Ultrafine PdAg alloy nanoparticles anchored on NH2-functionalized 2D/2D TiO_(2) nanosheet/rGO composite as efficient and reusable catalyst for hydrogen release from additive-free formic acid at room temperature

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Journal of Energy Chemistry 2021年第8期30卷 455-464,I0010页

作者： Xi Zhao Ping Dai Dongyan Xu Xumei Tao Xien Liu Qingjie Ge State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042China Shandong Provincial Key Laboratory Of Polymer Material Advanced Manufacturing Technology College of Electromechanical EngineeringQingdao University of Science&TechnologyQingdao 266061China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia University750021 YinchuanChina

A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal *** as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction *** from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.

关键词： formic acid Dehydrogenation TNS-rGO composite PdAg alloy Amine-functionalization