TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2024
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IF 4.7
Yi ZHANG,Han-xiao LIAO,Lu YANG,Bin-hua ZHOU,Xuan-zhi LIU,Huan-huan ZHAI,Xiao-rong HE,Hong-jun HUANG,Peng-fei TAN,Jun PAN
In order to address the issue that the photocatalytic reduction of hexavalent chromium (Cr(VI)) is often limited by the inefficient utilization of electrons in photocatalysts, a quasi-MOF photocatalyst using thiocyanate (—SCN) was developed as a modulator to enhance the charge transfer properties of ZIF-L-based photocatalysts. The incorporation of —SCN introduced structural defects, which improved visible light absorption and the reduction ability of photogenerated electrons. —SCN significantly adjusted the electronic properties and established a stable electron release pathway, serving as active sites for reduction. The optimized quasi-MOF demonstrated a Cr(VI) reduction rate of 94.8% in neutral potassium thiocyanate solution under visible light without a hole scavenger. The reaction rate constant is 2.8 times that of the photocatalyst without defect modulation. This study offers a promising strategy for developing highly efficient photocatalysts for environmental remediation.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Zuo-Shu Sun,Xue-Yan Xiang,Qiu-Ping Zhao,Zhao Tang,Shi-Yi Jiang,Tong-Bu Lu,Zhi-Ming Zhang,Baifan Wang,Hua-Qing Yin
Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@ n C- T ( n represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and T = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis via NO 3 − and CO 2 co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h −1 g FeNi −1 with a Faradaic efficiency of 15.56% at –1.2 V vs . RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2024
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IF 4.7
Shuai LI,Sheng-hai YANG,Yong-ming CHEN,Chao-bo TANG,Yan-qing LAI,Chao-yong DENG,Chang-hong WANG
Electrodissolution-coupled hafnium alkoxide synthesis (EHS) is a promising pathway for efficient electro- synthesis. It employs simultaneous heterogeneous reactions of Hf dissolution and ethanol dehydrogenation, and spontaneous solution-based combination reaction between Hf 4+ cations and alkoxy anions. To elucidate the mechanism and kinetics of EHS process, the electrochemical behaviors of anodic Hf dissolution and cathodic ethanol dehydrogenation were explored through electrochemical measurements, SEM observations, gas chromatography, and micro-kinetics modeling. The results indicated the supporting electrolytes of tetraethylammonium chloride (Et 4 NCl) to be preferable, which facilitated a passive-film-punctured pitting mechanism for Hf dissolution and a two-stage dehydrogenation mechanism. Three indicators related to passive rate, sensitivity towards puncture of the passive film, and pitting rate were extracted to quantify the kinetics of passive puncture and Hf corrosion. Micro-kinetics models were developed to evaluate the Et 4 NCl-based EHS process, which achieved electric energy requirements of 1.53–1.83 kW·h/kg Hf(OC 2 H 5 ) 4 .
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Bo Zhang,Ru Xiao,Liyuan Liu,Xiaobin Liu,Ying Deng,Qingliang Lv,Zexing Wu,Yunmei Du,Yanyan Li,Zhenyu Xiao,Lei Wang
Although the intermittent energy-driven direct seawater splitting technology provides an unparalleled approach to achieving sustainable development, the severe corrosion via aggressive Cl – severely affects the stability and efficiency of the anode catalyst and limits its industrial application. Herein, a lattice Cl – functioned NiFe-LDH electrode (E-NF-LDH Cl or E-NF-LDH SW ) is firstly constructed by a minute-level electrochemistry assisted chlorine corrosion strategy, which presents enhanced oxygen evolution reaction (OER) performance and excellent anti-Cl – corrosion behavior for seawater splitting. The optimized E-NF-LDH Cl and E-NF-LDH SW deliver low OER overpotential of 355 and 384 mV to reach 1 A cm −2 current density in the 1 mol L –1 KOH and 1 mol L –1 KOH seawater, respectively, as well as excellent stability of E-NF-LDH Cl is maintained at 1 A cm –2 for 400 h in the 1 mol L –1 KOH and 1 mol L –1 KOH + 0.5 mol L –1 NaCl. MD (molecular dynamics) simulation and DFT (density functional theory) calculation confirmed that strong common-ion repulsion effect in IHP region repels free Cl – , forming high spin polarization centers and more single electrons to enhance the intrinsic activity of OER.
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高影响因子
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2024
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IF 4.7
Qiang WANG,Meng WANG,Zong-yu FENG,Yong-qi ZHANG,Xiao-wei HUANG,Xiang-xin XUE
For a highly efficient recycling of a wastewater containing a high concentration of MgCl 2 , Al(III) and P507 were scheduled to be removed in advance. In this study, the in-situ removal of Al(III) and P507 from a high concentration MgCl 2 solution at different pH values and Al/P molar ratios was investigated. The results showed that P507 formed organic complexes of Al x (OH) z + y -P507 at pH of 2.0−4.0. At pH of 4.0−5.0, Al(III) precipitated and transferred into Al(OH) 3 with a flocculent amorphous morphology. Active sites on the Al(OH) 3 surface enhanced the removal efficiency of P507. At pH of 6.0−6.5, Al(III) and Mg(II) formed layered crystalline Al(OH) 3 and MgAl 2 (OH) 8 with small pore channels and fewer active sites, resulting in a reduced removal efficiency of P507. When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0, the removal rates of both Al(III) and P507 were higher than 98%, while the concentration loss of Mg(II) was only 0.2%−0.9%.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Hongyu Qu,Wende Hu,Xiangcheng Li,Rui Xu,Xiao Han,Junjie Li,Yiqing Lu,Yingchun Ye,Chuanming Wang,Zhendong Wang,Weimin Yang
Selective hydrogenolysis of biomass-based platform compounds is of great importance for the production of chemicals and fuels. Herein, we reported that the catalyst of Ni-C 3 N 4 supported on H 2 activated carbon (HC) synthesized by a simple coordination-impregnation-pyrolysis method is efficient for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF); the yield of 94.2% can be obtained in a batch reactor and the lifetime of greater than 120 h can be achieved in fixed-bed experiment. It is demonstrated that Ni nanoparticles coated by graphitic C 3 N 4 shell were highly dispersed on the surface of HC and the Ni loading is as low as 0.86 wt%, beneficial to the anti-sintering of Ni nanoparticles during the reaction. Both XPS characterizations and theoretical calculations reveal that Ni 3 N is the intrinsic active component for the hydrogenolysis , which exhibits efficient activity for the dissociation of C–O bond. This work opens up a new avenue to develop catalysts with single non-noble metal component for the efficient conversion of biomass-based chemicals.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Xiang Zhang,Weihang Li,Jin Zhang,Haoshen Zhou,Miao Zhong
Electrochemical nitrate (NO 3 − ) reduction offers a promising route for ammonia (NH 3 ) synthesis from industrial wastewater using renewable energy. However, achieving selective and active NO 3 − to NH 3 conversion at low potentials remains challenging due to complex multi-electron transfer processes and competing reactions. Herein, we tackle this challenge by developing a cascade catalysis approach using synergistic active sites at Cu-Fe 2 O 3 interfaces, significantly reducing the NO 3 − to NH 3 at a low onset potential to about +0.4 V RHE . Specifically, Cu optimizes *NO 3 adsorption, facilitating NO 3 − to nitrite (NO 2 − ) conversion, while adjacent Fe species in Fe 2 O 3 promote the subsequent NO 2 − reduction to NH 3 with favorable *NO 2 adsorption. Electrochemical operating experiments, in situ Raman spectroscopy, and in situ infrared spectroscopy consolidate this improved onset potential and reduction kinetics via cascade catalysis. An NH 3 partial current density of ~423 mA cm −2 and an NH 3 Faradaic efficiency (FE NH3 ) of 99.4% were achieved at −0.6 V RHE , with a maximum NH 3 production rate of 2.71 mmol h −1 cm −2 at −0.8 V RHE . Remarkably, the half-cell energy efficiency exceeded 35% at −0.27 V RHE (80% i R corrected), maintaining an FE NH3 above 90% across a wide range of NO 3 − concentrations (0.05−1 mol L −1 ). Using 15 N isotopic tracing, we confirmed NO 3 − as the sole nitrogen source and attained a 98% NO 3 − removal efficiency. The catalyst exhibit stability over 106-h of continuous operation without noticeable degradation. This work highlights distinctive active sites in Cu-Fe 2 O 3 for promoting the cascade NO 3 − to NO 2 − and NO 2 − to NH 3 electrolysis at industrial relevant current densities.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2024
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IF 4.7
Xiao-qing LU,Ai-min LIU,Feng-guo LIU,Xian-wei HU,Zhong-ning SHI
The feasibility and reaction mechanism of NdFeB film electrodeposition in 1,3-dimethyl-2-imidazolidinone (DMI)−LiNO 3 ionic liquid analogs at room temperature were investigated. Cyclic voltammetry indicated that the reduction peak at −1.83 V (vs Ag) was related to the reduction of Fe(II) to Fe, while the reduction peak at −2.01 V (vs Ag) was related to the reduction of B(III) to B. The electrochemical reduction reaction of Fe(II) and B(III) were irreversible processes controlled by diffusion, and the diffusion coefficients of Fe(II) and B(III) at 313 K were 3.03×10 −6 and 6.74×10 −7 cm 2 /s, respectively. In addition, XRD analysis suggested that the product obtained by the electrodeposition in DMI−LiNO 3 −Nd(CF 3 SO 3 ) 3 −FeCl 2 −H 3 BO 3 ionic liquid analogs for 2 h on the Al substrate contained NdFe 3 B 3 . SEM and EDS analysis showed that Nd, Fe, and B in the cathode product were uniformly distributed. XPS analysis revealed that the mass fractions of Nd, Fe, and B on the W substrate were 27.44%, 27.90%, and 7.51%, respectively.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Jingya Guo,Wei Liu,Wenzhe Shang,Duanhui Si,Chao Zhu,Jinwen Hu,Cuncun Xin,Xusheng Cheng,Songlin Zhang,Suchan Song,Xiuyun Wang,Yantao Shi
Endowing metal-free graphitic carbon electrodes with high electrocatalytic reactivity is a field of intense research, but remains elusive. Here, we introduce a prototypical edge-plane-site-specific engineering strategy on “herringbone” multi-walled carbon nanotubes by performing an intercalation-exfoliation and truncation process in molten inorganic salts. Controllable synthesis of the target H-MWCNTs-MS with fully exposed edge-plane sites on both the outer surface and inner channels was demonstrated. in-situ infrared spectroscopic study supports the theoretically energetic “edge-state” and identifies the reconstructed ketone/carboxyl-terminated edge sites under oxygen evolution reaction (OER) conditions. These oxygenated edge-plane sites boost charge redistribution and interlayer coupling, which essentially govern the synergistic catalysis, as evidenced by combined theoretical, electrokinetic, and H/D isotopic studies. Benefiting from the dense reactive sites and efficient electron tunneling, the H-MWCNTs-MS demonstrated impressive OER activity with an overpotential of 236 mV at a current density of 10 mA cm −2 in alkaline media, outperforming most state-of-the-art metal-free electrocatalysts reported to date. Furthermore, the catalyst displayed no noticeable degradation during 100 h of operation, indicating its potential for practical applications.
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高影响因子
NEW CARBON MATERIALS
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2024
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IF 6.5
Xiao-li Yan,Kui Wang,Shu-wei Hao,Guang-da Zhou,Hao-wei Yang,Hua Zhang,Jun-jie Guo
Exploring cost-efficient and highly-efficient noble metal-free catalysts for the oxygen reduction reactions (ORRs) involved in sustainable energy devices remains a great challenge. Transition-metal phosphides supported on heteroatom-doped carbons have shown potential as alternative candidates for precious metals because of their tunable electronic structures and higher catalytic performance. Phosphating was used to construct CoP nanoparticles (NPs) anchored on a nitrogen-doped porous carbon framework (CoP@NC) from Co NPs loaded on NC, using PH 3 gas released from NaH 2 PO 2 during heat treatment. The dodecahedral structure of Co NPs was retained in their transformation to CoP NPs. The CoP@NC electrocatalyst shows a remarkable ORR activity with a half-wave potential up to 0.92 V under alkaline conditions, which is attributed to the combined coupling between the well dispersed CoP nanoparticles on the nitrogen-doped carbon and the efficient mass transport in the porous structure. Zinc-air batteries assembled with the CoP@NC electrocatalyst as a cathode have a high open-circuit voltage of 1.51 V and power density of 210.1 mW cm −2 . This work provides a novel strategy to develop low-cost catalysts with an excellent ORR performance to promote their practical use in metal-air batteries
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Zhaoping Shi,Ziang Wang,Hongxiang Wu,Meiling Xiao,Changpeng Liu,Wei Xing
The development of high-performance oxygen evolution reaction catalysts with low iridium content is the key to the scale-up of proton exchange membrane water electrolyzer (PEMWE) for green hydrogen production. Single-site electrocatalysts with maximized atomic efficiency are held as promising candidates but still suffer from inadequate activity and stability in practical electrolyzer due to the low site density. Here, we proposed a NaNO 3 -assistant thermal decomposition strategy for the preparation of high-density Ir single sites on MnO 2 substrate (NaNO 3 -H-Ir-MnO 2 ). Direct spectroscopic evidence suggests the inclusion of NaNO 3 accelerates the transformation of Ir-Cl to Ir-O coordination, thus generating uniform dispersed high-density Ir single sites in the products. The optimized H-Ir-MnO 2 demonstrates not only high intrinsic activity in a three-electrode set-up but also boosted performance in scalable PEMWE, requiring a cell voltage of only 1.74 V to attain a high current density of 2 A cm ‒2 at a low Ir loading of 0.18 mg Ir cm ‒2 . This work offers a new insight for enhancing the industrial practicality of Ir-based single site catalysts.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
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IF 15.7
Mengran Liu,Canyu Liu,Tianfang Yang,Shixiang Hu,Siyun Li,Shizhe Liu,Yang Liu,Ye Chen,Bingcheng Ge,Shuyan Gao
Transition metal Ni anchored in carbon material represents outstanding 2e − oxygen reduction reaction (ORR) catalytic selectivity, but enhancing the adsorption strength of intermediate *OOH to promote its selectivity remains a major challenge. Herein, the NiX/Ni@NCHS composite catalyst with heteroatom doping (O,S) is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni. With the synergistic effect of honeycomb structure and O atom, NiO/Ni@NCHS-700 exhibits an exceptional H 2 O 2 selectivity of above 89.1% across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte, and an unexpected H 2 O 2 production rate up to 1.47 mol g cat ‒1 h ‒1 @0.2 V, which outperforms most of the state-of-the-art catalyst. Meanwhile, NiS/Ni@NCHS exhibits excellent electrocatalytic performance, with 2e − ORR selectivity of 91.3%, H 2 O 2 yield of 1.85 @0.3 V. Density functional theory simulations and experiments results reveal that the heteroatom doping (O,S) method has been employed to regulate the adsorption strength of Ni atoms with *OOH, and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site. The heteroatom doping method in this work provides significant guidance for promoting 2e − ORR electrocatalysis to produce H 2 O 2 .
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