Catalysts
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2024
·Vol. 14
·期 10
·683
·
IF 3.8
Deqin He,Zheng Liang,Juwen Gu,Xuechun Sang,Yujia Liu,Songbai Qiu
Furfuryl alcohol represents a pivotal intermediate in the high-value utilization of renewable furfural, derived from agricultural residues. The industrial-scale hydrogenation of furfural to furfuryl alcohol typically employs Cu-based catalysts, but their limited catalytic activity necessitates high-temperature and high-pressure conditions. Here, we develop robust CuNi bimetallic catalysts through direct calcination of dried sol–gel precursors under H2atmosphere, enabling the complete conversion of furfural to furfuryl alcohol under mild conditions. By adjusting the calcination atmosphere and introducing small amounts of Ni, we achieve the formation of highly dispersed, ultrasmall Cu nanoparticles, resulting in a significant enhancement of the catalytic activity. The optimized 0.5%Ni-10%Cu/SiO2-CA(H2) catalyst demonstrates superior catalytic performance, achieving 99.4% of furfural conversion and 99.9% of furfuryl alcohol selectivity, respectively, at 55 °C under 2 MPa H2, outperforming previously reported Cu-based catalysts. The excellent performance of CuNi bimetallic catalysts can be attributed to the highly dispersed Cu nanoparticles and the synergistic effect between Cu and Ni for H2activation. This research contributes to the rational design of Cu-based catalysts for the selective hydrogenation of furfural.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Shaomin Zhou,Xi Zhang,Lulu Zhan,Xianliang Song,Rui Li,Yulong Wu
Furfural (FF) is an important platform chemical that can be produced from lignocellulosic biomass rich in xylan. However, the traditional one-step FF production process produces a large amount of residue rich in sulfuric acid, approximately 15 tons per ton of FF. In this study, a carbon-based solid acid catalyst ZnCS-2 was developed for the two-step catalytic conversion of lignocellulosic biomass to FF. Furfural yields of up to 72.4 % were obtained at 180 °C for 60 min with 10 wt% catalyst ZnCS-2 catalyst. Using this catalytic system, a conceptual process for a two-step FF production system (TSF) was established. With the aim of performing a quantitative comparison with traditional production, a one-step FF production process (OSF) simulation alongside a lifecycle analysis was performed. Comparing the two-step method with the traditional one-step method, the advantages and disadvantages of the two methods and the direction of improvement can be systematically analyzed. The results demonstrated that the TSF process, which employs the ZnCS-2 catalyst and a biphasic solvent system of MIBK/NaCl, achieved a higher furfural yield. Specifically, the final yield of the TSF process exceeded that of the OSF process by 49.9 %. For every ton of furfural produced, the TSF process resulted in reductions of 0.07 kg SO 2 eq, 186.15 kg CO 2 eq, 1 × 10 −5 kg CFC-11 eq, and 66.13 kg 1,4-DB-eq in emissions compared with OSF. Owing to the higher yield and sulfur-free corncob residue, the profitability of TSF process was found to be 6.75 times greater than that of the OSF process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Weichen Wang,Hongke Zhang,Fangyuan Zhou,Yidan Wang,Zhiyu Xiang,Wanbin Zhu,Hongliang Wang
Developing cost-effective and highly active catalysts for the selective hydrogenation of furfural to target products is significant yet remains a substantial conundrum in the chemical industry. Herein, we present a phytic acid-assisting pyrolysis strategy to phase-controlled synthesis of a series of nickel phosphides catalysts (Ni 3 P/mSiO 2 , Ni 12 P 5 /mSiO 2 and Ni 2 P/mSiO 2 ), which exhibited phase-dependent catalytic performance in furfural hydrogenation. Ni 12 P 5 /mSiO 2 achieved the highest yield (97.3 %) of cyclopentanone under 1 MPa H 2 at 150 °C, and Ni 3 P/mSiO 2 could further hydrogenate cyclopentanone to a 60.8 % yield of cyclopentanol when the H 2 pressure increased to 2 MPa. Meanwhile, Ni 2 P/mSiO 2 demonstrated temperature-controlled selectivity for switching between furfuryl alcohol and cyclopentanone. Detailed characterizations and density functional theory calculations elucidated that the differences in catalytic performance were primarily attributed to the hydrogenation ability and acidity of catalysts as well as furfural adsorption configuration, which were determined by the tunable crystal phases of nickel phosphides. This work paves the promising avenue for the rational design of metal phosphide catalysts and harnessing their considerable potential for biomass conversion.
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ENERGY & FUELS
·
2024
·
IF 5.2
Jinbo Yang,Shengqi Lin,Chunhe Li,Kuankuan Ren,Qiufeng Ye,Weidong Dou
Utilizing photocatalytic technology to efficiently convert biomass-derived compounds into value-added chemicals and release hydrogen gas can effectively address energy and environmental issues. For this purpose, we fabricated a series of NiMoS4/Zn0.6Cd0.4S nanocomposites through a simple two-pot hydrothermal treatment. Dexterously, the photoexcited electrons and holes can be simultaneously utilized to participate in a photocatalytic redox reaction, effectively achieving the oxidation of furfuryl alcohol while cooperating with H2 evolution. The hydrogen evolution rate of 10%-NiMoS4/Zn0.6Cd0.4S nanocomposite in 1.50 vol % furfuryl alcohol aqueous solution is as high as 289.5 μmol·h–1, which is approximately 2895 and 41 times higher than that of pure NiMoS4 and Zn0.6Cd0.4S, respectively. Meanwhile, after 13 cycles of photocatalytic reaction, the conversion efficiency and selectivity of converting furfuryl alcohol to furfural are 68.5% and 94.0%, respectively. This photocatalyst also shows high photocurrent, low impedance, and efficient photogenerated carrier separation and transport properties, which can be attributed to the establishment of an ohmic junction between NiMoS4 and Zn0.6Cd0.4S. It is anticipated that this work can provide inspiration for the effective conversion of biomass-derived platform chemicals into high-value chemicals through visible-light-driven photocatalytic technology.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Wei Lv,Yao Wang,Hong Chen,Yongqi Tang,Yongdan Li
Nitrogen atom-doped biomass carbon prepared from corn stover is a newly discovered metal-free catalyst that shows good activity on the selective oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-diformylfuran (DFF). Here, the presence of graphitic nitrogen on the catalyst surface activated the oxygen adsorbed on the carbon sites next to the graphitic nitrogen in the carbon material and promoted the formation of oxygen radicals on the surface-active sites, improving the HMF oxidation process. The results show that the catalyst NC-800 reacted with acetonitrile as the reaction solvent at 110 °C and 1.0 MPa O 2 for 8 h to obtain 93.0 % HMF conversion and 94.4 % DFF selectivity, and the 5-HMF conversion and DFF selectivity were maintained at more than 85 % after five cyclic tests, with excellent cyclic stability. One of the main factors influencing the material flaws is the variation in pyrolysis temperature. Using maize stover, a readily available and renewable biomass, in the catalytic oxidation of biomass platform compounds may improve biomass utilization more extensively.
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BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Zonghui Liu,Xueting Zhu,Chao Cai,Jiayi Zheng,Bing Yan,Liangmin Ning,Dan Yang,Bing Xue
Developing conversion routes from lignocellulosic platform compounds to high-value chemicals is fundamental to advancing sustainable resource utilization in the bioeconomy. In this study, we designed a series of SBA-15-supported bifunctional catalysts with precisely tunable Lewis acid sites (LAS), Brønsted acid sites (BAS), and basic sites through strategic incorporation of hafnium species and heteropolyacids (HPAs), demonstrating their exceptional performance in the multi-step tandem conversion of furfural (FUR) to γ-valerolactone (GVL). HfO 2 was used LAS and basic sites to catalyze the transfer hydrogenation reaction of FUR and levulinate ester using 2-propanol as the H-donor. Complementary to this, HPA could catalyze the hydrolytic ring-opening of furans. The amount of LAS, BAS, and basic sites was adjusted by changing the ratio of HPA to HfO 2 and the types of HPA (phosphotungstic acid (HPW), phosphomolybdic acid (HPMo), silicotungstic acid (HSiW) and silicomolybdic acid (HSiMo)). The ratio of HPA to HfO 2 and types of HPA have a great influence on the catalytic performance, among which HPW/Hf-SBA-15_0.37 (W/Hf = 0.37) was identified as the best catalyst and presented the highest GVL selectivity (73.5 %) under optimized reaction conditions. The poison experiment (addition of benzoic acid, pyridine, or 2,6-lutidine to the reaction) indicated that both acidic and basic sites play important role in the FUR to GVL reaction. Moreover, by correlating the catalyst performance with the BAS/LAS ratio of catalysts, it can be found that the balance between the BAS and LAS is also the key to higher GVL selectivity.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Van Nho Tran,Quoc-Nam Ha,Dong-Hau Kuo
Biomass-derived molecules, as renewable sources of organic carbon, are essential for selectively transforming into valuable chemicals and fuels, aiding in the mitigation of the energy dilemma brought on by the depletion of traditional fossil fuels. Owing to its unique chemical structure, furfural (FFR) is widely regarded as a key platform molecule derived from biomass, capable of being converted into various valuable chemicals, such as 2-furoic acid (2-FA). In this study, we design a CuWCe trimetal-doped Ni₃S₂ thin-film electrocatalyst that incorporates multivalent cations (Cu + /Cu 2+ , W 5+ /W 6+ , and Ce 3+ ) to enhance the economic feasibility of electrocatalytic FFR conversion to 2-FA for commercial use. We successfully synthesized an in situ grown nanoflower-like CuWCe-2 electrocatalytic material using a simple hydrothermal method. The catalyst achieved an FFR conversion efficiency of 79.8% to 2-FA, with a selectivity of 89.6%, at an FFR initial concentration of 35 mM. The 2-FA was produced at a high yield rate of 876 μmol·cm -2 ·h -1 and a faradaic efficiency (FE) of 90.1% at 1.45 V versus the reversible hydrogen electrode (RHE) in an H-cell setup.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yanping Dong,Xiqiang Tian,Muhammad Zahid
Due to their highly tunable structures and porous nature, metal-organic frameworks (MOFs) have garnered substantial interest as versatile platforms for immobilizing noble metal nanoparticles in selective hydrogenation catalysis. However, the inherent limitations of MOFs, such as small micropores and weak interactions between inorganic nodes and guest noble metals (caused by organic ligands), often result in limited accessibility and the collapse of reactive sites. To overcome these challenges, this study focuses on a novel partial deligandation strategy and further, stabilizes the active Pt nanoparticles over it. Specifically, Ti-MOF-250 was synthesized by partially decomposing NH 2 –Ti-MIL-125 (Ti-MOF) at 250 °C, followed by the eco-friendly polyol reduction method to produce Pt/Ti-MOF-250 catalyst. Compared to the non-deliganded Ti-MOF, the Ti-MOF-250 catalyst, which retains residual organic ligands, exhibits a greater surface area, a hierarchical porous structure, and active defect sites that expose the unsaturated Ti metal centers. These features synergistically control the Pt particle size, enhance their uniform dispersion, and increase the number of exposed reactive sites. The distinctive structural properties of the Pt/Ti-MOF-250 catalyst enable unique furfural (FAL) adsorption geometries, achieving exceptional FAL conversion (97.4 %) and high selectivity (98.1 %) toward furfuryl alcohol (FOL). The partial deligandation approach paves the way to enhance the physicochemical properties of pristine MOFs, enabling the homogeneous confinement and stabilization of Pt nanoparticle catalysts to achieve exceptional catalytic activity, selectivity, and stability in hydrogenation reactions.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Honghui Gong,Fei Wang,Qi Li,Longxing Wei,Juan Zhang,Yuan Ma,Yifan Rui,Xian-Lei Shi
Selective synthesis of cyclopentanol (CPL) from biomass-derived furfural (FAL) is highly attractive, but it still faces serious challenges. In this work, an alloyed Cu–Co catalyst derived from Cu–Co–Al layered double hydroxide (LDH) was grafted onto sulfur-doped coffee biochar for the first time (Cu–Co–Al/SCB). Cu–Co–Al/SCB achieved a maximum CPL yield of 97.5% and a high turnover frequency (TOF) of 15.6 h–1 in the selective hydrogenative rearrangement of FAL at 140 °C. The characterization results demonstrated that grafting Cu–Co–Al onto SCB results in the formation of Cu–Co alloys and a strong interaction between them. Further characterization and activity tests demonstrated that the formation of a highly dispersed Cu–Co alloy and in situ generated Brønsted acid sites collaboratively catalyzes the selective hydrogenative rearrangement of FAL to CPL over Cu–Co–Al/SCB, and the strong interaction between the Cu–Co alloy and sulfur-doped coffee biochar endowed Cu–Co–Al/SCB with remarkable stability. As a result, Cu–Co–Al/SCB is a promising catalyst for the selective hydrogenative rearrangement of FAL.
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ACS Catalysis
·
2025
·
IF 13.1
Yang Li,Jian Zhang,Wei Zhang,Chang Zhou,Jianbin Huang,Zerui Su,Ziyuan Qiao,Xiaoyuan Qin,Pei Xiong,Feng-Shou Xiao
Direct hydrogenolysis of biomass-derived furfural to produce 1,5-pentanediol, an essential precursor for polyesters and polyurethanes, plays a significant role in biomass utilization. In this work, using the carbothermal shock strategy, 1.5PtCo1Ce1-CTS ternary metal oxides were successfully prepared, containing abundant oxygen vacancies (Ov) and Co2+ species that are favorable for hydrogen transfer and ring-opening of furan, thereby enhancing catalytic activity and 1,5-pentanediol selectivity. Under an optimized condition (170 °C, 3 MPa of H2, 4 h), the 1.5PtCo1Ce1-CTS catalyst achieved furfural conversion at 99.3% and 1,5-pentanediol selectivity at 59.2%. During recycling tests, the 1.5PtCo1Ce1-CTS catalyst exhibited high resistance to deactivation with a simple and rapid regeneration process. This work offers an alternative, versatile, and eco-friendly strategy for designing efficient heterogeneous catalysts for the hydrogenolysis of furfural into 1,5-pentanediol in the future.
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FUEL
·
2025
·
IF 7.5
Yutong Zhu,Guohua Miao,Yucheng Hu,Ning Yan,Tingting You,Haq Nawaz,Zhen Wu,Feng Xu
Ni-based catalysts show promise in valorization of bio-based aldehydes. Designing an efficient and stable Ni-based catalysts for bio-conversion still remains a significant challenge. In this work, a sustainable, simple, and solvent-free method was developed to synthesize Ni x Zn@CNT catalyst with unique active phase Ni 3 ZnC 0.7 encapsulated in carbon nanotubes (CNT). The amount of active phase was regulated by varying Ni/Zn doping content. The as-obtained Ni 4 Zn@CNT (Ni/Zn ratio is 4:1) demonstrated excellent catalytic activity for furfural hydrogenation, yielding 99% conversion and 86.75% selectivity to furfuryl alcohol (FAOL). Density functional theory (DFT) calculations, XRD, and Py-FTIR analyses demonstrated that the activation of FAOL and H 2 was synergistically enhanced by the formed Ni 3 ZnC 0.7 phase and Ni 0 . Benefiting from the encapsulation of the active phase uniformly in CNT, Ni 4 /Zn@CNT catalyst displayed outstanding reusability with more than 98% of the furfural conversion even after reuse for six times, thereby outperforming most reported Ni-based catalysts. The method developed in this study provides a sustainable approach for preparing highly durable and efficient Ni-based catalysts for hydrogenation reaction.
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CELLULOSE
·
2018
·Vol. 25
·期 7
·3843-3851
·
IF 3.809
Hu Hui-Chao,Zhang Yu,Zeng Tong,Zhou Weining,Chen Lihui,Huang Liulian,Ni Yonghao
This paper reports a robust method for rapid determination of cellulose derived 5-hydroxymethyl-2-furfural (5-HMF) in biomass hydrolysate suspension based on headspace gas chromatography (HS-GC). The headspace equilibration at 150 °C for longer than 4 min with a pH range of 2.0–3.5 and a 50% (v/v) of ethanol content can obtain the full evaporation of 5-HMF, and eliminate the formation of additional 5-HMF generation from hexose. The linear GC response of 5-HMF was achieved by controlling the sample size within 20 μL. The results showed that this method has a good precision (relative standard deviation < 6.97%) and accuracy (recoveries ranged from 94.0 to 104.8%). The limit of quantification of the method was 51 mg/L. It was also found that a considerable amount of furfural (13.8%) and 5-HMF (18.7%) was adsorbed on condensed lignin and humins in residual biomass, and the washing procedure with ethanol can completely extract the adsorbed furfural and 5-HMF. The present method is accurate, simple, and robust, it will be a powerful tool for determining the content of 5-HMF in the liquid samples from biorefinery related processes.
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