Molecular Catalysis
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2018
·
IF 0
Zhongzhe Wei,Xuefeng Li,Jiang Deng,Jing Wang,Haoran Li,Yong Wang
The catalytic transformation from levulinic acid (LA) into γ-valerolactone (GVL) is of great interest as it is an impressive strategy to convert lignocellulosic platform chemical into high value-added compounds. Herein, a novel heterogeneous catalyst made of Ru nanoparticles (NPs) supported on N-doped hierarchically porous carbon from biomass, Ru/NHPC, was shown to be highly active, selective and stable in this transformation. The reaction can proceed smoothly under mild conditions in aqueous media even at room temperature. The catalyst Ru/NHPC could be recycled for 13 consecutive runs exhibiting no obvious activity decay, much better than that of Ru NPs supported on activated carbon. The process offers an efficient, environmentally responsible, and safe approach to high production of GVL.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Dong-Ning Li,Ai-Jun Wang,Jie Wei,Qian-Li Zhang,Jiu-Ju Feng
Herein, we developed a facile one-pot co-reduction method to fabricate highly dentritic platinum-palladium/palladium core-shell nanocrystals on reduced graphene oxide (PtPd@Pd NCs/rGO), where poly- l -lysine (PLL) worked as the eco-friendly structure director and stabilizer . The nanocomposite was mainly characterized by microscopic analysis, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and thermogravimetric analysis (TGA), along with the discussion of the formation mechanism. The synthesized PtPd@Pd NCs/rGO have the enlarged electrochemically active surface area (ECSA) of 51.65 m 2 g −1 , showing 1.3 folds enhancement in the peak current density relative to commercial Pt/C (50 wt%) for glycerol oxidation reaction (GOR), coupled with the small Tafel slope of 28 mV dec −1 for hydrogen evolution reaction (HER).
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Kelong Ao,Dawei Li,Yixin Yao,Pengfei Lv,Yibing Cai,Qufu Wei
Heteroatom doping is a feasible approach to adjust catalytic performance of the HER catalysts. In this work, we report a design of Fe-doped Co 9 S 8 nanosheets grown on carbon cloth (Fe-Co 9 S 8 NSs/CC) as a hydrophilic 3D monolithic electrocatalyst for efficient hydrogen evolution under all pH. The water contact angle and electrochemical measurements proved that the resultant material was hydrophilic for its nano hierarchitectures and dopant Fe enhanced the catalytic capability of singular Co 9 S 8 . In 1.0 M KOH, the Fe-Co 9 S 8 NSs/CC possessed a relatively small Tafel slope (95.3 mV dec −1 ) and required the overpotential of 83 mV to achieve 10 mA cm −2 . To drive the same current density, the overpotentials were 65 and 192 mV in 0.5 M H 2 SO 4 and 1.0 M PBS, respectively. Meanwhile, it showed good cycle stability and durability over 20 h static test at alkaline and neutral condition. The flexible freestanding catalyst has great potential in practical applications.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Li Yan,Lu Lijun,Jiang Xueyu,Yang Dali,Chen Jeng-Lung,Dutta Chowdhury Abhishek,Li Wu,Pei Xianglin,Lei Aiwen
Biomass valorization is a way to promote the ‘waste-to-wealth’ concept, which is a pre-requisite condition for a future sustainable lifestyle. The direct utilization of natural polymer for value-added materials should be prioritized. With this object, we demonstrate a facile and economical method to prepare chitin-derived supramolecular nanowires-stabilized single-atom sites Pt catalysts (SS-Pt-CSNs). A comprehensive characterization shows the structure of single-atom Pt coordinated with the organic supramolecular (ligand-type) entity, which is both flexible (like in homogenous catalyst) and robust (like in heterogenous catalyst). Such hybrid characteristics of these SS-Pt-CSNs materials exhibit excellent catalytic performance for chemo-selective hydrogenation of various unsaturated bonds with a selectivity of more than 90:1 and a high turnover number (TON) of 121,350. Mechanistic studies demonstrate that both empty coordination sites of Pt and dynamic B-doping are the key factors for exceptional efficiency and high selectivity.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Zhenjie Ma,Xiangshang Chen,Gaoyang Zhou,Yue Jia,Huayan Chen,Xiaolong Lu
A stability-enhanced extraction gel membrane (EGM) with a thin functional layer of carrier for metal ion recovery was prepared and improved by cross-linking technology. Hydroxyl-terminated polybutadiene (HTPB) was used as the coupling agent to form a cross-linked network skeleton. Polymethylhydrosiloxane (PMHS) and HTPB were hydrosilylated to form a compact cross-linked structure. In addition, the D2EHPA (carrier) was fixed on polymer cross-linked structure. The prepared stability-enhanced EGM was characterized by SEM, EDS, ATR-IR, XPS . The influence of preparation parameters was studied and compared systematically. The optimum preparation conditions obtained from the data indicate that the total polymer concentration is 8 wt%, the mass ratio of HTPB/PMHS is 1:2, and the mass ratio of TEOS/VTES is 1:1. After 72 h of stability experiments, the mass transfer flux decreased from 2065.46 mg m −2 h −1 –1718.82 mg m −2 h −1 , the overall flux attenuation rate is only 16.8 %, which is 50.8 % lower than that of EGM without surface enhancing layer. In comparison, the flux attenuation rate of the traditional supported liquid membrane (SLM) even reached 100 % after 66 h. Therefore, the stability-enhanced EGM prepared in this study presents obviously higher operating stability compared with the EGMs operated at same conditions. The results suggest a potential approach for metal ions removal from water with high efficiency and stability.
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Catalysts
·
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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Qiaohong Su,Qingcui Liu,Pengyue Wang,Juan Ding,Jiulin Wang,Yudai Huang
High overpotential and low stability are major challenges for hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). Tuning the electronic structure of catalysts is regarded as a core strategy to enhance catalytic activity. Herein, we report CuO x /Cu nanorod skeleton supported Ru doped cobalt oxide/nitrogen-doped carbon nanocomposites (Ru-CoO/NC/CuO x /Cu, denoted as RCUF) as bifunctional catalysis. The one-dimensional/three-dimensional (1D/3D) nanostructure and defect-rich amorphous/crystalline phases of RCUF facilitates active site exposure and electron transport. Experimental characterization and density functional theory (DFT) calculation results indicate that Ru doping can optimize the electronic structure, which accelerates the water dissociation process and reduces the Gibbs free energy of the reaction intermediates. As expected, the optimal RCUF-900 exhibits low overpotential (25/205 mV at 10 mA cm −2 ) and high stability (100/100 h) for HER/OER. RCUF-900 has low voltage (1.54 V at 10 mA cm −2 ) and high stability (100 h) for overall water splitting. This work provides new insights into the design of advanced catalysts for overall water splitting.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Jiajin Li,Minglei Lu,Yuxin Ge,Weiwei Lu,Zidi Liu,Hongde Xu,Yu Zhang,Zhihui Li,Zhuoyu Zheng,Pengxiang Gao,Qian Zhang,Tiejun Wang
Aqueous-phase reforming of methanol (APRM) is an important method for H 2 production, widely used in energy fields like polymer electrolyte membrane fuel cells (PEMFCs). However, traditional noble metal catalysts , being expensive and vulnerable to CO poisoning, restrict their practical application. Therefore, developing robust non-noble metal catalysts for efficient and sustainable H 2 production with low CO levels in APRM at low temperatures is highly significant. In this study, a novel approach was employed to synthesize carbon-encapsulated Cu catalyst via controlled pyrolysis , leading to Cu@CA-Val catalyst with excellent low-temperature catalytic activity. The optimal Cu@CA-Val-300 catalyst exhibited a high hydrogen production rate of 0.2–27.0 μmolH 2 /g cat /s over a wide temperature of 135–180 °C (base-free), surpassing the most Cu-based and Pt-based catalysts. The Cu@CA-Val-300 catalyst exhibited exceptional hydrothermal stability during continuous operation in a fixed reactor for 200 h. Efficient H 2 production was attributed to good wettability , enabling the diffusion of CH 3 OH and H 2 O molecules into Cu + /Cu 0 sites for activation, with CO being suppressed and transformed through the formate formation.
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International Journal of Minerals Metallurgy and Materials
·
2024
·Vol. 32
·期 2
·476-487
·
IF 5.6
Chen Junkang,Zhuang Yongyue,Qiao Yanxin,Zhang Yu,Yuan Aihua,Zhou Hu
Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for developing rechargeable zinc-air batteries (ZABs). Herein, an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere (NCS) decorated with dual-phase Co/Co 7 Fe 3 heterojunctions (CoFe@NCS). The phase composition of materials has been adjusted by controlling the alloying degree. The optimal CoFe 0.08 @NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm −2 for OER in an alkaline electrolyte. The intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co 7 Fe 3 alloy and metallic Co species. When the CoFe 0.08 @NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery (ZAB), the device shows a high peak power-density (157 mW·cm −2 ) and maintains a stable voltage gap over 150 h, outperforming those of the benchmark (Pt/C+RuO 2 )-based device. In particular, the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending conditions. Our work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Chaoran Pi,Difei Leng,Xuming Zhang,Shuangjie Wu,Yun Li,Li Huang,Zhihong Liu,Paul K. Chu,Kaifu Huo
The self-reconstruction of electrocatalysts during the cathodic hydrogen evolution reaction (HER) has garnered significant interest due to its impact on microstructure and electrocatalytic efficiency. Understanding the mechanisms driving this transformation is crucial for the development of high-performance HER pre-catalysts. In this study, an efficient Co(OH) 2 (001)/MoN (002) heterostructured catalyst is fabricated through the self-reconstruction of the Co/MoN pre-catalyst and the mechanism of facet-induced reconstruction is investigated in detail. This Co/MoN pre-catalyst exhibits an impressive 58 % reduction in overpotential at a constant current density of 100 mA cm −2 over 5 h. It ultimately achieves a low overpotential of 339 mV at 1 A cm −2 , outperforming commercial Pt/C under similar current conditions, while maintaining high current activity with 99.4 % retention after 110 h of continuous electrolysis. Operando characterizations and theoretical simulations reveal that metallic Co dissolves rapidly under bias as H + ions infiltrate the interstitial spaces, and the dissolved Co 2+ ions preferentially deposit as Co(OH) 2 nanosheets. This deposition aligns with the (001) facet of Co(OH) 2 and the prominent (002) plane of the MoN matrix through lattice matching, exhibiting a very low interfacial formation energy. Density-functional theory analysis reveals that the alignment of the crystal facets between Co(OH) 2 (001) and MoN (002) enhances electron transfer and modulates the interface to boost the water dissociation and hydrogen adsorption activity and kinetics. Our results underscore the importance of precise control over the reconstruction process for cathodic HER and facilitate the development of advanced transition metal-based electrocatalysts for industrial alkaline hydrogen production.
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Advanced Energy Materials
·
2024
·
IF 24.4
Yalei Fan,Xubin Ye,Jing Zhou,Dabiao Lu,Chang-Yang Kuo,Yu-Cheng Huang,Ting-Shan Chan,Chien-Te Chen,Youwen Long,Jian-Qiang Wang,Zhiwei Hu,Linjuan Zhang
Electrochemical water-splitting is vital in energy storage and conversion applications. However, the sluggish kinetics of the oxygen evolution reaction (OER) hinders the electrochemical water-splitting. Therefore, developing efficient catalysts and understanding the OER mechanism are highly desirable. This study successfully synthesized a new quadruple perovskite oxide CaCu 3 Co 2 Ru 2 O 12 (CCCRO) catalyst exhibiting high OER activity with overpotential 198 mV at 10 mA cm −2 , a Tafel slope of 37 mV dec −1 , and long-term operational stability with a current density of 500 mA cm −2 for >500 h. The in situ X-ray absorption near-edge structure (XANES) indicated that a part of high-spin (HS) Co 3+ ions and low-spin (LS) Ru 5+ ions transitioned to the tetravalent Co (IV) and hexavalent Ru (VI) valence states under OER. However, the Cu 2+ valence state remained unchanged. Furthermore, the density functional theory (DFT) calculations reveal that the lattice-oxygen oxidation mechanism (LOM) rather than conventional adsorbate evolution mechanism (AEM) is responsible for high OER activity in Ru (VI)-O-Co (IV) network, and that the Cu(A’)/Co(B)/Ru(B’) three sites synergistically facilitate the OER activity for CCCRO.
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FUEL
·
2024
·
IF 6.7
Shi Chen,Yueqi Zhao,Caiyun Chang,Xinyi Wang,Li Hou,Jing Jin,Faming Gao
The low electron transfer efficiency compared to precious metals, few active sites and poor stability of transition metal sulfides (TMSs) limit their wide application in electrocatalysis. Optimizing the electronic structure and morphology is an effective means to improve the catalytic performance of TMSs. In this work, we synthesized a heterogeneous core–shell CoFeMo polymetallic sulfide/N-rich carbon skeleton composite catalyst (CFMS/NC) with CoMo-S as the core and CoFeMo-S as the shell by using MOF as precursor and stepwise substitution method. Compared with monomeric sulfides, polymetallic sulfides can exert the synergistic effect between metals, optimize the electronic structure and improve the intrinsic activity of metallic sulfides. Meanwhile, the core–shell structure supported by N-rich carbon skeleton has larger active specific surface area, higher stability and conductivity. The overpotential of CFMS/NC catalyst is only 122 mV at 10 mA cm −2 for hydrogen evolution reaction (HER) and 325 mV at 50 mA cm −2 for oxygen evolution reaction (OER). Besides, CFMS/NC exhibits outstanding performance in overall water splitting, achieving a current density of 100 mA cm −2 at only 1.76 V and maintaining good stability for 30 h. This study proposes a practical method for synthesizing highly efficient electrocatalysts for water splitting.
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