Reaction Chemistry & Engineering
·
2020
·Vol. 5
·期 5
·886-895
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IF 3.441
Xing-Gang Si,Yun-Peng Zhao,Qing-Lu Song,Jing-Pei Cao,Rui-Yu Wang,Xian-Yong Wei
A highly efficient Ni/N–C catalyst was synthesized by facile pyrolysis of a Ni-containing metal–organic framework (Ni-MOF), and its catalytic hydrogenolysis performance towards C–O bonds in lignin was evaluated in detail using diphenyl ether (DPE) as a model compound. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analyses show that the flower-like nanosheets of the Ni-MOF shrink, forming a loose and ordered spherical structure during pyrolysis. Under the optimal conditions, DPE was completely converted and the selectivity to monomers (benzene, cyclohexanol and cyclohexane) reached 99.1%. During the catalytic hydrogenolysis conversion (CHC) of DPE, the direct cleavage of the Caromatic–O bond affording benzene and phenol is the major reaction pathway, and a low H2 pressure is crucial to increase the monomer selectivity. Furthermore, Ni/N–C-450 shows high hydrogenolysis activity for other lignin-derived aryl ethers, such as benzyl phenyl ether, dibenzyl ether, dinaphthalene ether, benzyl 2-naphthyl ether and 3-methoxyphenol.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xue Zhang,Chunxia Wu,Ye Bu,Ying Liang,Zhitong Wang,Jing Li,Daoxiong Wu,Xinlong Tian,Peilin Deng
Exploring efficient and durable methanol oxidation reaction (MOR) electrocatalysts is crucial for the industrialization of direct methanol fuel cells. Herein, we designed MOR electrocatalyst of PtRu/Ni-N-C, in which PtRu nanoclusters (PtRu NCs) are loading on nitrogen-doping carbon support anchoring Ni single atoms (Ni-N-C). Compared with PtRu NCs and Pt/C, PtRu/Ni-N-C exhibits more excellent MOR activity with 2050 mA mg pt -1 and tougher anti-CO toxicity over 6000 s CA test, proving that the synergetic effect of nanoclusters and single atoms support enhance MOR activity and resistance to anti-CO toxicity. The fine spectroscopy analysis and density functional theory (DFT) calculations demonstrate that the strong metal-support interaction (SMSI) between nanoclusters and single atoms, facilitating the electron transfer of about 0.4 e from PtRu NCs to the Ni-N-C support, effectively reduces the d -band center of Pt to weaken the adsorption capacity of *CO and *COOH intermediates. Moreover, the synergistic sites derived PtRu NCs coupling Ni single atoms accelerate *OH adsorption, promoting the adjacent *CO removal. This work offers deep insight into the SMSI effect between nanoclusters and single atoms support to design the efficient Pt-based MOR electrocatalysts.
研究领域:
材料科学
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电化学
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催化
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ping Zhang,Hao Chen,Lin Chen,Ying Xiong,Ziqi Sun,Haoyu Yang,Yingke Fu,Yaping Zhang,Ting Liao,Fei Li
Atomically dispersed catalytic metal sites anchored on N-doped carbon support catalysts (M-N-C) show great prospects for CO 2 electroreduction. Here, single-layer NiZn layered double hydroxides (NiZn-LDHs) was used as a sacrificial assistant to fabricate single-Ni atom anchored on ultrathin porous carbon catalyst. NiZn-LDHs were exfoliated to single-layer by polyhydroxy compounds which took as the carbon resource in Ni-N-C, and single layer NiZn LDHs taking as the Ni resource could avoid the agglomeration of Ni atoms during calcining. The CO Faradaic efficiency (FE CO ) of the synthesized Ni-N-C catalyst exceeded 90% at −0.6 to −1.0 V and a FE CO of 95.2% with a current density of 24 mA cm −2 at −0.9 V. This work not only provides a new method for preparing M-N-C catalysts, but also offers an effective and controllable strategy for large-scale production of high-performance single-atom catalysts.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhicheng Liu,Manli Wang,Ming Hou,Yun Zhao,Wenbin Yang,Yangkai Han,Zhigang Shao
In traditional CO 2 electrolysis systems, oxygen evolution reaction (OER) consumes 90 % of the electricity input, whereas the product of oxygen holds minimal value. Moreover, the use of different electrocatalysts for the anode and cathode remains a challenge due to high capital costs of the electrolysis system. Substituting the OER with thermodynamically advantageous value-added anodic reactions and developing bifunctional electrocatalysts are crucial for the advancement of CO 2 electrolysis. In this study, for the first time, we present an innovative CO 2 electrolysis system that integrates CO 2 electroreduction reaction (CO 2 RR) with SO 2 electrooxidation reaction (SO 2 OR) and employ Ni-N-C as the bifunctional electrocatalysts to produce CO and H 2 SO 4 simultaneously. Notably, the novel CO 2 electrolysis system can reduce the cell voltage by 1.05 V, resulting in nearly 50 % reduction in energy consumption. This is also the first attempt to use Ni-N-C to catalyze SO 2 OR, showing markedly superior performance compared to commercial 20 % Pt/C. In-situ ATR-SEIRAS and DFT calculations demonstrate that the NiN 4 sites in Ni-N-C catalysts augment the direct conversion of *SO 2 to *HSO 4 - , identified as the rate-determining step for the SO 2 OR. This work provides guidance for the design of novel CO 2 electrolysis systems, the construction of bifunctional electrocatalysts, as well as the mechanistic investigation of the SO 2 OR.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
ChemSusChem
·
2023
·
IF 8.4
Jiaji Zhang,Gaobo Lin,Jie Zhu,Sifan Wang,Wenhua Zhou,Xiangzhou Lv,Bolong Li,Jianghao Wang,Xiuyang Lu,Jie Fu
Graphical We find that the N-doped Ni particles can enhance the adsorption of CO 2 and modulate the configuration of adsorbed CO on Ni-N-C sites. As a result, the optimal catalyst can efficiently convert CO 2 into CO with a faradaic efficiency of 96.7 % and a current density of 500 mA cm −2 in a strongly acidic electrolyte. Electro-chemically reducing CO 2 in a highly acidic medium is promising for addressing the issue of carbonate accumulation. However, the hydrogen evolution reaction (HER) typically dominates the acidic CO 2 reduction. Herein, we construct an efficient electro-catalyst for CO formation based on a core-shell structure, where nitrogen-doped Ni nanoparticles coexist with nitrogen-coordinated Ni single atoms. The optimal catalyst demonstrates a significantly improved CO faradaic efficiency (FE) of 96.7 % in the acidic electrolyte (pH=1) at an industrial-scale current density of 500 mA cm −2 . Notably, the optimal catalyst maintains a high FE of CO exceeding 90 % (current density=500 mA cm −2 ) in the electrolyte with a wide pH range from 0.67 to 14. In-situ spectroscopic characterization and density functional theory calculations show that the local electron density of Ni-N-C sites is enhanced by N-doped Ni particles, which facilitates the formation of *COOH intermediate and the adsorption of *CO. This study demonstrates the potential of a hybrid metal/Ni-N-C interface in boosting acidic CO 2 electro-reduction.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
PubMed
高影响因子
Green Chemical Engineering
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2022
·
IF 0
Jianguo Liu,Jiangmin Sun,Thishana Singh,Shanshan Lin,Longlong Ma
Although precious transition metals such as palladium, platinum, and iridium are widely used in hydrogenation reactions, the earth-abundant transition metal-catalyzed highly selective semi-hydrogenation of terminal alkynes to terminal alkenes remains poorly developed and a challenge. Herein we demonstrate the excellent selective, cost-effective semi-hydrogenation of terminal alkynes via a novel graphene encapsulated Ni@N/C catalyst. The graphene layer encapsulated nano-catalyst Ni@N/C could significantly avoid metal leaching and improve the stability of the catalyst. The strong interaction of nitrogen with the Ni nanoparticles regulates the activity of Ni towards selective semi-hydrogenation of terminal alkynes. Substrates having un-functionalized as well as functionalized substituents, and substrates having sensitive functional groups (olefins, ketones) which pose a challenge to hydrogenate, were semi-hydrogenated with excellent conversion (up to 99%) and selectivity (up to 99%) under optimized reaction conditions.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 35
·14970-14978
·
IF 3.288
Jingchuang Zhao,Yingzhen Zhang,Xianyu Kang,Yancai Li
Direct methanol fuel cells (DMFCs) have been extensively studied for developing a new non-precious metal catalyst to replace commercial platinum catalysts, due to their expensive cost and susceptibility to CO poisoning. In this work, nanocomposites of nickel oxide/nickel supported by N-doped carbon (NiO/Ni–N/C) were prepared by using a hydrothermal method and further carbonization at different temperatures. The surface morphology and composition of the NiO/Ni–N/C nanocomposites were characterized by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). As observed through electrochemical experiments, the NiO/Ni–N/C nanocomposite modified glassy carbon electrode (NiO/Ni–N/C/GCE) exhibits high electrocatalytic activity for the methanol oxidation reaction (MOR) in alkaline solution. Among the nanocomposites, NiO/Ni–N/C carbonized at 500 °C (NiO/Ni–N/C500) displays the highest mass activity (1043 mA mgNi−1) at 0.73 V (vs. Ag/AgCl), which is much higher than that of Ni(OH)2/N–C and NiO/Ni–N/C carbonized at other temperatures (400, 600, and 700 °C). In addition, the catalytic activity of NiO/Ni–N/C500 is 2.12 times that of the commercial Pt/C. NiO/Ni–N/C500/GCE also possesses fast kinetics, excellent stability and CO tolerance. Therefore, the NiO/Ni–N/C500 nanocomposites have great application potential as MOR catalysts.
研究领域:
材料科学
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电化学
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纳米技术
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催化
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2022
·Vol. 69
·期 2
·e17877
·
IF 4.167
Tianjin Li,Bo Chen,Meifang Cao,Xinping Ouyang,Xueqing Qiu,Changzhi Li
The efficient utilization of lignin remains a great challenge due to its complex nonrepetitive structure and the lack of efficient catalyst. Herein, a single-atom catalyst Ni@N-C was designed via a facile chelation-anchored strategy. Ni atoms were immobilized on the N-doped carbon carrier by a two-stage pyrolysis of a mixture of d -glucosamine hydrochloride, nickel acetate, and melamine. d -glucosamine hydrochloride as a chelating agent prevented the aggregation of Ni 2+ , and melamine provided enough N to anchor Ni by forming Ni–N 4 structure. Ni@N-C gave a 31.2% yield of aromatic compounds from lignin hydrogenolysis, which was twice higher than that achieved by Ni cluster catalyst. Based on the experimental and density functional theory (DFT) calculation results, the higher activity of Ni@N-C was attributed to its lower H 2 dissociation energy and the reduced energy barriers of the transition states. The strategy described opens an efficient green avenue for preparing single-atom catalyst that possesses outstanding activity in lignin depolymerization.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Jiage Yu,Wei Liu,Lu Bai,Benqiang Tian,Qingyi Zhu,Qianxi Yang,Linlin Zhou,Haoyang Wu,Yuan Wang,Boyuan Li,Xiangrong Jin,Yun Kuang,Jiazhan Li,Xiaoming Sun
CO 2 electroreduction typically requires large overpotentials to sustain high reaction rates, which at current densities approaching 1 A cm −2 inevitably intensify competition from the hydrogen evolution reaction (HER), making it difficult to simultaneously sustain high product selectivity (>95%). In this study, hollow Ni─NC (H-Ni-NC) was synthesized using nanoscale silica sphere templates and atomic Zn as a sacrificial pore-former within the carbon shell. The optimized H-Ni-NC achieves a current density of −1.0 A cm −2 with over 95% CO Faradaic efficiency in a flow cell. The high performance was attributed to the hollow sphere architecture enriched with gas-permeable through-pores. Notably, the Zn dosage selectively modulates the shell through-porosity, without altering hollow sphere macrostructure or the active-site structure, thereby enabling a systematic investigation of porosity effects. Finite-element simulations provide a qualitative framework suggesting a trade-off between reactant transport and active surface area with increasing porosity in hollow spherical catalysts. This work underscores that engineering of the nanoscale mass-transport environment surrounding active sites plays a critical role in designing high-efficiency electrocatalysts.
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产品关联
DOI
PubMed
高影响因子
Chemistry-An Asian Journal
·
2024
·
IF 3.5
Yicheng Wang,Qiyu Zhang,Chenxu Wang,Ayeza,Yating Zhang,Chao Hu
The utilization of renewable energy for electrocatalytic carbon dioxide reduction reaction (CO 2 RR) represents a pivotal technology in sustainable carbon conversion. Single-atom catalysts (SACs) featuring transition metal-nitrogen-carbon (M−N−C) structures have demonstrated exceptional electrocatalytic efficacy in CO 2 RR by maximizing atom efficiency. Nevertheless, further investigation is warranted to optimize the catalytic performance of SACs through the selection of suitable carbon sources and supports, as well as the modulation of the microenvironment surrounding individual metal atoms. In this study, a sulfur-doped Ni−N−C catalyst was prepared using a two-step strategy involving metal ion adsorption and thermal decomposition, with porous ion exchange resin serving as the carbon source. Due to the uniform distribution of single atom active centers on the resin-based carbon support and sulfur doping, this catalyst efficiently converts CO 2 into CO with a Faradaic efficiency exceeding 90 % within the range of −0.69~−1.29 V (vs. RHE), reaching a maximum value of 97.7 % (−0.79 V vs. RHE). Theoretical calculations indicate that second-shell sulfur doping effectively promotes coupled transfer of protons and electrons, leading to a significant reduction in Gibbs free energy barriers for CO 2 RR intermediate products.
研究领域:
材料科学
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电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Liquan Xiong,Ying Wang,Di Gao,Yueqi Song,Dongsheng Chen
Hydrogen energy is the core of future clean energy, and the study of hydrogen evolution reaction (HER) electrocatalytic mechanisms is essential for efficient production. The development of efficient and low-cost electrocatalysts is a key challenge in achieving ideal hydrogen generation. In this study, a Ni-BDC/TpPa-1 heterojunction material was prepared for the first time, which was converted into a derived heterojunction material (NiO@Ni/N-C) after high-temperature pyrolysis treatment, exhibiting excellent electrocatalytic activity in an alkaline solution. Without iR compensation, the overpotential of HER is only 83 mV at a current density of 10 mA·cm⁻². Compared with thermally decomposed Ni-BDC and TpPa-1 monomer, its electrocatalytic activity is improved by 158 and 435 mV, respectively, and it exhibits excellent stability over 100 h. The design of this novel material offers a new solution for enhancing the efficiency of transition-metal-based catalysts.
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DOI
高影响因子
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