NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 8
·6381-6388
·
IF 3.201
Guoqiang Liu,Xian Zhang,Cuijiao Zhao,Qizhong Xiong,Wanbing Gong,Guozhong Wang,Yunxia Zhang,Haimin Zhang,Huijun Zhao
Electrocatalytic water splitting as an environmentally friendly method to produce clean H2 has attracted wide attention. However, efficient improvement of the performance of the oxidation half-reaction during water splitting, thus enhancing H2 evolution efficiency, has become an urgent issue. Herein, non-precious metal Co0.83Ni0.17 alloy nanoparticles on activated carbon (Co0.83Ni0.17/AC) have been successfully fabricated by a simple thermal-treatment method. The resulting Co0.83Ni0.17/AC with a dominant alloy particle size of 45 nm exhibits a microporous and mesoporous structure with a surface area of 159.2 m2 g−1. As an electrocatalyst, the as-prepared Co0.83Ni0.17/AC demonstrates bifunctional electrocatalytic activity toward the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline media, delivering overpotentials of 193 and 325 mV at 10 mA cm−2, respectively. Importantly, it is found that the electrocatalytic oxidation of benzyl alcohol to benzoic acid on Co0.83Ni0.17/AC is more favourable than the OER process, with almost 224 mV less overpotential at 10 mA cm−2 and 96% faradaic efficiency at 1.425 V vs. RHE (passing charge amount of ∼40C). As a simultaneous anode and cathode electrocatalyst for water splitting, Co0.83Ni0.17/AC displays a H2 generation rate of 8.98 μmol min−1 in 1.0 M KOH solution containing 10 mM benzyl alcohol, almost 1.4 times that obtained by an OER-introduced water splitting system, with near 98% faradaic efficiency for H2. This work would be helpful to develop low-cost and abundant bifunctional electrocatalysts for electrocatalytic organic synthesis and simultaneously improving H2 generation from water splitting.
研究领域:
化学工程
·
材料科学
·
可再生能源
✓ 已验证
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 7
·1064
·
IF 3.9
Yutong Ye,Guorong Zhou,Kaixun Li,Yun Tong
Anion modification and trace metal doping have been widely demonstrated to have unique advantages in regulating both electrocatalytic activity and the electronic structure of non-precious metal materials. Developing a simple and practical preparation strategy is critical, but it still faces challenges. In this paper, a novel type of dual-modification approach is put forward to rationally design the S, Pt-CoNi material, which can be grown directly on the nickel foam (NF) in a one-step electrodeposition process. The multiple advantages of having plenty of active sites, high conductivity, and a faster charge transfer endow the optimized reaction kinetic for HER. The prepared S, Pt-CoNi/NF catalyst displays excellent catalytic performance, and a low overpotential of 116 mV at 50 mA cm−2and a small Tafel slope of 75 mV dec−1are achieved. The coupled S, Pt-CoNi/NF||FeOOH/NF electrolyzer delivers a high current density of 100 mA cm−2at the potential of 1.61 V as well as superior stability under alkaline conditions. Our work experimentally confirms the feasibility of constructing a dual-regulation strategy via one-step electrodeposition, and it also provides ideas for the controllable design of other high-performance electrodes for electrocatalysis.Keywords:dual-modification;CoNi alloy;electrodeposition;electrocatalytic hydrogen production;alkaline medium
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 2
·113
·
IF 3.8
Hongzhi Ding,Chenyu Yang,Congyan Jiang,Wei Luo,Qiuyue Wang,Xuefeng Guo
The use of eco-friendly biomass as a resource is an efficient way to address the problems of fossil fuel depletion and climate change. In biomass conversion, versatile γ-valerolactone (GVL) is generally obtained from levulinic acid (LA) hydrogenation via a multimetallic catalyst system. Despite conversion efficiency being enhanced in mild conditions due to metal interactions, maintaining high catalyst stability is still a challenge. In this study, we synthesized a surrounded Co0.52Ni0.48@Al2O3-IE catalyst that exhibited excellent alloying and synergistic interaction between the metal constituents. Under relatively mild reaction conditions, the GVL yield over the catalyst exceeded 99% in LA hydrogenation. The catalyst showed no deactivation in a test of five cycles, displaying superiority in stability, possibly due to reasons of the physical isolation of the shell and the alumina retention on the Co-Ni alloys surface caused by the reversibility of exchange equilibrium. The present work demonstrated that a surrounded structured catalyst fabricated by ion exchange (IE) with active metals physically enclosed can lead to high catalytic activity and superior stability.
研究领域:
催化化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 20
·3194-3201
·
IF 4.568
Jun Wu,Xinyue Yan,Wenrui Wang,Ming Jin,Yuhang Xie,Chengbing Wang
Graphical Efficient, stable, and low-cost N-doped graphitic carbon embedded CoNi bimetallic alloy nanocatalysts were developed for the catalytic transfer hydrogenation of biomass-derived furfural to value-added furfuryl alcohol with isopropanol as hydrogen donor. The synergy enabled by bimetallic alloys and abundant N-based Lewis-base sites and surface Co−N active species were responsible for the excellent catalytic performance. The development of efficient, stable, and cost-effective heterogeneous catalysts for catalytic transfer hydrogenation (CTH) of biomass-derived furfural (FAL) is highly desired. Herein, series of N-doped graphitic carbon embedded CoNi bimetallic alloy nanoparticles were fabricated and used for the CTH of FAL to value-added furfuryl alcohol (FOL) with renewable isopropanol as hydrogen donor. Intrinsic catalytic activity examination indicated the catalytic performance of Ni x Co y @NGC (x:y=1 : 3, 1 : 1, 3 : 1) nanocatalysts were sensitive to their chemical compositions. The optimal Ni 1 Co 1 @NGC nanocatalyst with Ni/Co mole ratio of 1 : 1 afforded a largest FOL yield of 89.3% with nearly full conversion of FAL. The synergistic effect enabled by bimetallic alloys and the abundant N-based Lewis base sites and surface Co−N active species were revealed based on systematic structural characterization, responsible for the excellent catalytic efficiency of bimetallic Ni 1 Co 1 @NGC nanocatalyst for CTH of FAL.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 47
·17499-17506
·
IF 4.052
Sihang Cheng,Yanchun Liu,Yingnan Zhao,Xinyu Zhao,Zhongling Lang,Huaqiao Tan,Tianyu Qiu,Yonghui Wang
Aromatic amino compounds are important and universally used chemical intermediates in a wide range of industrial fields. Thus, their production with high efficiency and selectivity under ambient conditions is expected and demanded in modern industry. Herein, a series of superfine CoNi alloy nanoparticles embedded in Al2O3 nanosheet (CoxNi1−x/Al2O3, where x represents the content of Co in the precursor) catalysts was fabricated from CoNiAl-LDH and used to catalyze the tandem dehydrogenation of ammonia borane (AB) and hydrogenation of nitroaromatics to the corresponding amines. Systematic experiments indicate that the composition, size, morphology and catalytic performance of the CoxNi1−x/Al2O3 catalysts can be easily controlled by changing the content of Ni in the CoNiAl-LDH precursor. Particularly, Co0.67Ni0.33/Al2O3 exhibited the best tandem catalytic performance among the six samples. This as-prepared catalyst not only showed a moderate turn-over-frequency value (TOF: 34.5 molH2 molCo0.67Ni0.33−1 min−1 at 298 K without base or additives) and relatively low activation energy (32.4 kJ mol−1) for the dehydrogenation of AB, but also superior catalytic activity (conversion yield reaching up to 100%) and selectivity (>99%) for the tandem reductive transformation of in excess of sixteen types of nitroaromatics to aromatic amines. Density functional theory (DFT) calculations suggest that the construction of the CoNi alloy optimized the electronic structure with respect to the pure component, promoting its activity for AB hydrolysis and nitroaromatics hydrogenation. Finally, the catalyst could be easily recycled using a magnet due to the magnetic properties of the Co0.67Ni0.33 alloy.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ying Ding,Chaoqun Li,Xiaoyue Zhang,Wei Chen,Xuebin Yu,Guanglin Xia
While lithium borohydride is one of the most promising hydrogen storage materials due to its ultrahigh hydrogen storage density, high thermodynamic stability, kinetic barriers, and poor reversibility, it is far from being used in practical applications. Herein, we prepare a cubic hollow carbon dodecahedron uniformly modified with a bimetallic CoNi alloy (CoNi/NC) for preserving the stable catalytic effect of CoNi alloys toward reversible hydrogen storage. It is theoretically confirmed that bimetallic CoNi alloys effectively weaken the B–H bonds of LiBH4 by extending their average length to 1.33, 0.09 and 0.04 Å longer than that of LiBH4 and LiBH4 under metallic Co, respectively. More importantly, the alloying of Co with Ni avoids the reattachment of H from LiBH4 to the Co surface, which prevents LiBH4 from dehydrogenation for the formation of H2 on the Co surface, thus resulting in an ultralow hydrogen desorption energy of 0.1, 1.85 and 0.52 eV lower than that of LiBH4 and LiBH4 under metallic Co. Therefore, the onset and peak hydrogen desorption temperatures decrease to 130 and 355 °C, respectively, 170 and 97 °C lower than that of bulk LiBH4. More importantly, a reversible H2 capacity of 9.4 wt % is achieved even after 10 cycles.
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Zhibin Liu,Xiuping Sun,Zhirong Sun
Developing highly efficient, stable, recyclable, and application value heterogeneous catalysts in advanced oxidation processes has essential application value in the degradation of refractory pollutants. In this paper, the CoNi alloy anchored onto N-doped porous carbon (CoNi-600@NC) catalyst was prepared using bimetallic doped metal-organic frameworks as precursors. The magnetic CoNi-600@NC can activate peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). Therefore, SMX can be removed 100% within 25 min. CoNi-600@NC/PMS has a broad pH (3–9) application range, good applicability, and repeatability. Radical quenching, quantitative and electrochemical experiments proved that the degradation of SMX was dominated by free radical (Superoxide anions) and non-free radical pathways (surface-bound radicals). Mechanistic analysis showed that the interaction between Co-N x /pyridine N-sites and graphitized carbon with PMS induced the formation of surface-bound active species. Moreover, CoNi nanoparticles promoted the redox cycle of metals. The synergistic catalytic mechanisms between the CoNi alloy and the abundant functional groups gave CoNi-600@NC excellent catalytic properties and applicability. Using density functional theory predicted the reaction sites of SMX and proposed four degradation pathways. The toxicity of intermediates was comprehensively evaluated. In addition, a CoNi-600@NC continuous flow reactor was constructed with a daily treatment capacity of 45 L and 100% SMX removal. This study expands the application of persulfate advanced oxidation technology by synthesizing recyclable magnetic catalysts and provides new synergistic degradation mechanisms for removing refractory organics.
研究领域:
环境科学
·
催化材料
·
污染治理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Yuehong Xie,Chao Feng,Yuan Guo,Shiang Li,Cheng Guo,Yi Zhang,Jide Wang
This paper introduces a facile strategy to fabricate trifunctional electocatalysts through one pool treatment on MOFs to obtain carbon nanotube coated ultrafine CoNi alloy (CoNi@NCNTs) nanocomposites with N-doped rich-defect and abundant cavity structure. During the pyrolysis process, volatile CNx species from dicyandiamide were trapped by ZIF-67@Ni-ZIF nanosheets, simultaneously introducing nitrogen atom into carbon matrix to achieve the rich-defect porous nanotubes and abundant cavity structure. The as-prepared nanomaterials can simultaneously boost the ORR, OER and HER catalytic activity with strong durability. Significantly, the CoNi@NCNTs-700 exhibits excellent electrocatalytic activity including half-wave potential (E ORR, 1/2 ) of 0.80 V, lower operating voltage (E OER, 10 ) of 1.60 V at 10 mA cm −2 and potential difference (ΔE) of 0.80 V between E OER, 10 to E ORR, 1/2 in 0.1 M KOH, and low overpotential (E HER, 10 ) of −0.130 V reaching 10 mA cm −2 in acidic medium. The remarkable activity is ascribed to defect-rich porous carbon nanotubes structure and the synergistic effect between CoNi alloy nanoparticles, N-dope carbon and CoNi-Nx. And hollow structure facilitates to improve conductivity and stability. This work offers a useful archetypical template to design and construct efficient and stable trifunctional electrocatalysts, illustrating its viability for practical applications of energy conversion and storage devices.
研究领域:
材料科学
·
电化学
·
能源转换与存储
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yue Du,Zhiyi Zhong,Zhixian Shi,Lina Zhou,Song Pan,Xiaonan Xu,Yisi Liu,Dongbin Xiong,Kai Wang
The development of carbon-encapsulated alloy catalysts, through a rational design that integrates highly active Me-N-C sites, is essential for improving the reaction kinetics of both oxygen reduction (ORR) and oxygen evolution reactions (OER). This advancement is pivotal for the progression of efficient rechargeable zinc-air batteries (RZABs). In this study, we investigates a CoNi alloy decorated N-doped carbon nanotube (CoNi-NCNT) electrocatalyst using a dual-ligand strategy. Experimental characterizations and theoretical calculations reveales that the electronic modulation of the 3 d orbitals of the CoNi alloy by the CoN 3 sites enhances electronic conductivity during the ORR/OER process, leading to exceptional bifunctional activity. Electrochemical evaluations demonstrates the outstanding performances of CoNi-NCNT, with a half-wave potential of 0.81 V (versus RHE) for ORR and a low overpotential of 1.52 mV for OER at 10 mA cm −2 . Moreover, the CoNi-NCNT catalyzed Zn-air battery exhibits a remarkable specific capacity of 780 mAh g −1 and an exceptionally extended lifespan exceeding 800 h. This underscores the potential of this alloy strategy in the development of high-performance bifunctional ORR/OER electrocatalysts.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Chunjie Yu,Xingwu Zhai,Pengcheng Wu,Zhaoqing Zhu,Banghua Peng,Guixian Ge,Zhiyong Liu
Low cost, high activity and stability electrocatalysts for hydrogen evolution reaction (HER) have been extensively studied in recent years. We have successfully synthesized a transition metal phosphide electrocatalyst (CoNi@CP) with coating structure . The CoNi@CP was prepared with the mild conditions. An organophosphorus ligand was synthesized by simple organic reaction . It was synthesized by coordination with Co 2+ and Ni 2+ and then calcined. CoNi@CP has abundant and uniform phosphorus atom doping, no energy consumption in phosphating process, and avoids the generation of highly toxic gas PH 3 . Because of its special coating structure, the adsorption of H ∗ on its surface was enhanced, and the active center of CoNi was protected, which contributed greatly to the improvement of catalytic performance. At 10 mA/cm 2 current density, the overpotential of the catalyst only 74 mV, and the slope of Tafel was only 83 mVdec -1 . The performance of the catalyst remained unchanged after 1000 stability tests. In addition, we had proved theoretically that the catalyst had high HER activity by DFT calculation. Therefore, it provides inspiration for us to better develop efficient transition metal phosphide electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Mingliang Ma,Zijian Liao,Xuewei Su,Qixi Zheng,Yanyan Liu,Yan Wang,Yong Ma,Fei Wan
Increasing electromagnetic (EM) radiation has driven the rapid development of carbon-based EM wave absorption materials, but the design of light-weight and efficient carbon-based materials remains a huge challenge. Herein, N -doped carbon fibers embedded with CoNi alloy particles (CoNi/C fibers) were synthesized via electrospinning technology and carbonization . Then, conductive polypyrrole-coated CoNi/C fibers (CoNi/C@PPy composites) were synthesized by chemical polymerization. As-synthesized CoNi/C@PPy composites showed outstanding EM wave absorption property due to the synergistic effect between CoNi, N -doped carbon fibers and PPy. The optimal reflection loss (RL) is -68.78 dB (12.90 GHz) with the thickness of 2.43 mm and the low filler loading of 15 wt%. The widest effective absorption bandwidth (EAB) is 5.62 GHz with the thickness of 2.10 mm and the low filler loading of 20 wt%. The outstanding EM wave absorption property is mainly attributed to 3D network structure, great impedance matching and strong dielectric loss. The results showed that embedding magnetic alloy particles in carbon fibers coated with conductive polymers is an effective strategy for constructing efficient lightweight EM wave absorption materials.
研究领域:
材料科学
·
电磁工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COMPOSITES PART B-ENGINEERING
·
2021
·
IF 9.078
Jiajia Li,Jiaqi Qian,Xiaoyu Chen,Xiaoxi Zeng,Ling Li,Bo Ouyang,Erjun Kan,Wenming Zhang
A novel Co/Ni metal-organic framework (MOF)-derived three-dimensional (3D) nanoarchitecture in which graphene carbon-coated CoNi alloy nanoparticles grow on the tips of N-doped carbon nanotubes that are vertically-aligned on carbon nanofibers (Co/Ni@GC/NCNTs/CNFs) is fabricated. The Co/Ni@GC/NCNTs/CNFs electrode has a half-wave oxygen reduction reaction (ORR) potential of 0.80 V, a superior standing stability with 84.8% current retention after 175 000 s. The oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) reach a lower overpotential of 0.395 V and 0.15 V, respectively. Moreover, the resultant sample is an air cathode catalyst in a microbial fuel cell and indicates an utmost power density of 2100 ± 45 mW cm −2 , which is much better than that of the Pt/C electrode (1334 ± 61 mW m −2 ). The density functional theory calculation demonstrates that the designed Co/Ni@GC/NCNTs/CNFs catalyst can remarkably promote OER, ORR, and HER performance.
研究领域:
材料科学
·
电化学
·
纳米技术
·
催化
·
能源存储与转换
✓ 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）