APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Hui Su,Shaojia Song,Songsong Li,Yangqin Gao,Lei Ge,Weiyu Song,Tianyi Ma,Jian Liu
Rational design of low-cost and efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is imperative for renewable energy conversion. Herein, for the first time, a facile strategy is developed to synthesize M (M = Fe, Cu, Zn, Mo) doped bimetallic sulfide heterostructure Ni 3 S 2 /Co 3 S 4 electrocatalysts. The as-prepared bifunctional Cu-Ni 3 S 2 /Co 3 S 4 electrode exhibits excellent electrocatalytic activity for HER and OER in 1 M KOH electrolyte, and it requires only an overpotential of 79 mV (150 mV) to deliver 10 mA cm −2 (20 mA cm -2 ) current density for HER process. Moreover, it shows a considerable low cell voltage of 1.49 V at the current density of 10 mA cm -2 in a two-electrode configuration which is far surpassing most of the reported bifunctional metal sulfides. Meanwhile, besides increasing the specific surface area of the electrocatalyst by optimizing the microstructure, the introduction of Cu cation could also stimulate the formation of high-valent Ni/Co sites, which can be verified by XPS technique. Density function theory calculations demonstrate that the Cu-doping boosts the formation of high valent Co sites and enhances the charge transfer performance of Ni and Co species, thus promotes intrinsic catalytic activity through modulating the d-band center of Co and reducing the adsorption energy of H and O-containing intermediates (H*, OH*, OOH*) on the surface of the catalyst. This work suggests the importance of exploitation of transition metal ion-doping for promoting the electrocatalytic activity of bimetallic sulfides.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Wanfeng Xiong,Duanhui Si,Jundong Yi,Yuanbiao Huang,Hongfang Li,Rong Cao
Multicomponent heterogeneous catalysts present excellent catalytic performance attributed to the synergistic effect of multi-sites. Nevertheless, identifying the composition of the multi-sites and exploring the synergistic catalytic mechanisms for the multiple active sites in electrocatalytic CO 2 reduction reaction (CO 2 RR) still lack intensive study. This work regulates the chemical composition of Cu-based nanoreactors readily by adjusting the geometrical morphology of metal-organic frameworks precursor. The obtained cuboctahedron nanoreactor containing Cu-N 4 /Cu 2 O/Cu multiple active sites exhibits excellent CO 2 RR selectivity towards deep reduction product (80%) with high current density. Moreover, the tandem catalytic mechanism of multicomponent active sites has been studied intensively. The CO 2 molecule is firstly reduced in Cu-N 4 sites to form CO and then the CO is transfered to Cu 2 O/Cu sites for further deep reduction. The high concentration of CO provided by Cu-N 4 sites decreases the free energy of rate-determining step for CH 4 products in Cu 2 O sites. This work provides a promising direction for designing and synthesizing multicomponent Cu-based tandem catalysts to access high efficiency and selectivity in the electrocatalytic CO 2 reduction reaction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yuanli Li,Chunqiang Zhuang,Shi Qiu,Junfeng Gao,Quan Zhou,Zaicheng Sun,Zhenhui Kang,Xiaodong Han
Metal halide perovskites with broad optical absorption and long carrier lifetime are considered as ideal photocatalysts. However, their poor stability in water greatly impedes their application in photocatalytic H 2 evolution because they lose their crystalline structure in water. Herein, we proclaim a new class of photocatalysts: all-inorganic Cs-Cu-Cl perovskite quantum dots (QDs). It exhibits a high photocatalytic hydrogen production rate of ∼ 3.1 mmol/g/h without any cocatalyst under AM 1.5-G solar irradiation (100 mW/cm 2 ). Especially, it remains the high activity for up to 330 h without apparent deterioration of the hydrogen production rate. Density functional theory (DFT) calculations reveal that the Cu site works as the electron and proton absorption sites as the H 2 production active center. To our best knowledge, there is no report of metal halide perovskites as water-stable photocatalysts. This work opens an innovative way for guiding the exploration of metal halide perovskites photocatalysts for stable photocatalytic H 2 evolution.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Zichen Song,Xinxin Zhang,Jianqiu Zhu,Xiaolei Wang,Wenqian Wang,Xiangbo Ma,Jiantao Fu,Jian-Qiang Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
While copper complexes intrinsically provide Cu sites for electrocatalytic CO 2 reduction (ECR), their efficacy toward multicarbon products (C 2+ ) remains fundamentally limited by the operational instability of reactive Cu valence states and the inability to synchronously optimize *CO intermediate generation and C-C coupling within symmetric coordination environments. Herein, we judiciously design a single-crystal N, O co-coordinated copper complex (Cu(ICA) 2 ) featuring asymmetric N 2 -Cu-O 2 centers that precisely modulate the electronic structure and local adsorption environment. The Cu-N bonds stabilize partially reduced Cu δ⁺ sites while weakening Cu-O interactions, thus balancing structural integrity with catalytic reactivity. This asymmetric dual-site coordination concurrently hosts distinct *CO intermediates (atop-adsorbed *CO at Cu sites and bridge-adsorbed *CO at Cu-N sites), enabling cooperative C-C coupling into C 2 products. The catalyst achieves a record 69.2 % Faradaic efficiency for C 2 products at 400 mA cm −2 and 57.4 % for C 2 H 4 at 500 mA cm −2 in 1.0 M KOH, rivaling the state-of-the-art Cu-based complexes. In situ characterization and DFT calculations mechanistically corroborate that bridge-adsorbed *CO at Cu-N sites drives energetically favorable hydrogenation and C-C coupling pathways. This work establishes a coordination-asymmetry design principle for constructing robust molecular catalysts capable of efficient CO 2 -to-C 2+ conversion.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Junfei Wu,Qin Zhang,Zhuojun He,Yingli Zhang,Yangli Chen,Hai-Bo Liu,Jing Wang
Tetracycline antibiotics (TCs) are widely distributed in the environment owing to excessive usage and incomplete metabolic breakdown, posing significant risks to ecosystems and human health. Herein, a bifunctional material, Cu-TATB-PCA, was prepared for simultaneous adsorption and detection of TCs. The material was constructed using Cu-MOF as the structural scaffold, with 1-pyrenecarboxylic acid (PCA) grafted via a postsynthetic ligand exchange (PSE) approach. The incorporated PCA moiety functions as both an active site for enhanced adsorption capacity and a fluorescent reporter for sensitive detection. Cu-TATB-PCA demonstrated a remarkable adsorption performance toward TCs, with a maximum adsorption capacity of 520.8 mg/g for oxytetracycline (OTC), 473.9 mg/g for chlortetracycline, and 469.5 mg/g for tetracycline (TC). The high adsorption capacity was mainly attributed to the dominant role of π-π interactions, which worked synergistically with coordination bonds, electrostatic interactions, and hydrogen bonds to collectively contribute to the adsorption process. In addition, Cu-TATB-PCA exhibited a highly sensitive fluorescent response toward TCs due to the mechanism of inner filter effect, which achieved a detection limit of 0.586 μM for TC and 0.776 μM for OTC. The streamlined and efficient material design paradigm paves the way for the development of bifunctional adsorption-detection materials and offers a promising avenue for future research endeavors in this field.
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高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Hanjun Zhang,Jing Chen,Yuxin Shi,Yaoyue Yang,Xiaole Jiang
Regulating the local microenvironment of metal centers represents an effective yet challenging approach to enhance the catalytic performance of atomically dispersed transition metal-nitrogen-carbon (M–N–C) catalysts towards the oxygen reduction reaction (ORR). Herein, atomically dispersed Cu–N–C catalysts featuring with adjustable carbon vacancies/defects concentrations (Cu–N–C V –X) are fabricated using a simple molten-salt-assisted pyrolysis strategy. The optimized catalyst (Cu–N–C V -1000) exhibits superior ORR catalytic performance with a half-wave potential ( E 1/2 ) of 0.89 V versus the reversible hydrogen electrode (RHE) and a turnover frequency ( TOF ) of 5.01 e site -1 s −1 at 0.85 V, surpassing Pt/C and most recently reported single-atom catalysts. Theoretical calculations confirm that defects adjacent to Cu–N 3 site downshift the d-band center of active sites, facilitating the desorption of *OH intermediate and thereby significantly enhancing the ORR kinetics. Consequently, the Cu–N–C V -1000-based zinc-air battery (ZAB) delivers a peak power density of 175.0 mW cm −2 along with a high discharge specific capacity of 819.4 mA g -1 Zn . This work confirms that the deliberate creation of suitable defects is an effective approach to optimize the intrinsic ORR activity of atomic M–N x sites, providing new insights into the rational design of high-performance catalysts for practical metal-air batteries.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Lisong Zhong,Ying Li,Lirong Zheng,Jian Sun,Zhaohui Jin,Linqi Shi,Pengcheng Zhao,Baoyu Qi,Liu Yang,Zhongwei Chen
The development of highly active and robust non-noble-metal catalysts for alkaline hydrogen evolution reaction (HER) is imperative for industrial anion exchange membrane water electrolysis (AEMWE). Herein, we construct a hierarchically multiphase heterostructure via a customized reduction strategy, featuring uniformly dispersed Cu and Ni metallic phases anchored onto a conductive isolated MoO 2 substrate (Cu/Ni@MoO 2 ). The catalyst achieves an ultralow overpotential of 140.7 mV at 1 A cm −2 in 1 M KOH, coupled with ampere-level operational stability exceeding 2000 h without degradation. In-situ Raman spectroscopy and theoretical analyses unveil that Cu-mediated interfacial engineering dynamically restructures interfacial water networks, reduces the water dissociation barrier and optimizes hydrogen adsorption energy. Impressively, the AEMWE device equipped with a Cu/Ni@MoO 2 cathode achieves the industrial-relevant current densities 1.74 A cm −2 and 3.61 A cm −2 at the voltages of only 1.8 V and 2 V (60 °C), respectively, while demonstrating exceptional durability with negligible voltage decay throughout 1000 h operation at 0.5 A cm −2 . This work presents a novel design strategy for high-current-density electrocatalysts, bridging atomic-scale insights and industrial hydrogen production requirements.
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JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Peng Zhang,Guang-Hui Liu,Yao-Shun Wen,Yu-Hong Kang,Yang-Fan Yin,Sheng Li,Zhi-Xin Li,Zhi-Hao Ma
Morphology engineering plays a pivotal role in boosting catalytic performance over heterogeneous catalysis. However, although Y 2 O 3 (a rare earth oxide) has been found to possess various morphologies, including nanoplate (NP), nanosphere (NS) and nanorod (NR), the lack of understanding of its catalytic mechanism still limits its further application. Herein, catalytic mechanism of Y 2 O 3 morphologies in reverse water-gas shift (RWGS) reaction over Cu-based catalysts was systematically investigated. Although Y 2 O 3 morphologies don’t affect CO selectivity, it has a significant impact on CO 2 conversion and stability. Systematic characterization reveals that Y 2 O 3 morphologies not only can optimize the CO 2 adsorption capacity and Cu nanoparticles size to enhance catalytic activity, but also can regulate the metal-support interaction to improve catalytic stability. The order of activity and stability of the Cu/Y 2 O 3 catalysts from high to low is: Cu/ NP Y 2 O 3 > Cu/ NR Y 2 O 3 > Cu/ NS Y 2 O 3 . This work clarifies the morphological-performance relationship in rare earth oxide-Y 2 O 3 , providing a new approach for the design of high-performance Cu-based catalysts for RWGS reaction and promoting the application of morphology engineering in heterogeneous catalysis.
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CHEMICAL ENGINEERING COMMUNICATIONS
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2025
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IF 2
Lei Zhao,Xiaotong Dong,Haigang Zhou,Xu Wei,Zichao Yin,Zhikun Wang,Songqing Hu
To tackle the critical and multifaceted challenges of metal corrosion in oil and gas operations, a novel green corrosion inhibitor—copper-doped carbon dots (CuCDs)—was synthesized. The results demonstrate that CuCDs exhibit superior corrosion inhibition efficiency (84.20% at 150 mg/L) compared to non-copper-doped carbon dots (NCDs, 70.22% at 200 mg/L), with statistical significance confirmed by triplicate experiments (p < 0.05). Notably, CuCDs also show exceptional antibacterial activity against sulfate-reducing bacteria (SRB), achieving an 88% sterilization rate, which significantly mitigates microbial-induced corrosion. Electrochemical and surface analysis revealed that CuCDs form a denser protective layer on N80 steel, attributed to synergistic chemical and physical adsorption mechanisms. These findings highlight the dual-functional potential of CuCDs as a sustainable solution for simultaneous corrosion and microbial control in oilfield applications.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Weixin Li,Qing Liu,Zhongxuan Yin,Yongqing Ma,Ganhong Zheng,Chuhong Zhu,Zhenxiang Dai,Meiling Wang
The photocatalytic conversion of CH 4 into value added liquid products in high yield has always been a huge challenge due to unavoidable peroxidation. Here, a kind of Cu/ZnS/ZnO x -550 Z type heterojunction is designed for photocatalytic CH 4 oxidation into C1 products (including CH 3 OH, CH 3 OOH and HCHO) by O 2 through the synergistic catalysis of multiple mechanisms. The CH 4 photooxidation reaction at 30 °C yields 56 mmol g −1 of C1 oxygenated products during 8 h, which exhibits a much higher value than those reported in recent studies. In situ Fourier transform infrared spectroscopy, electron spin resonance spectroscopy, X-ray photoelectron spectroscopy, electrochemical measurements and density functional calculation are used to comprehensively clarify the underlying photocatalytic mechanism. It indicates that in situ formed singlet oxygen ( 1 O 2 ) not only plays vital roles in triggering CH 4 photooxidation to C1 products, but also suppresses products peroxidation by inhibiting ·OH formation. The incorporated Cu transforms the ZnS/ZnO heterojunction from type II to Z -scheme, enhances light absorption, and, together with oxygen vacancies, regulates the electronic structure of the catalyst, thereby facilitating the adsorption and dissociation of 1 O 2 , and ultimately achieving high efficiency of CH 4 photooxidation.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yanjun Wang,Yuancai Lv,Yifan Liu,Minghua Liu
The electrochemical reduction of nitrate for ammonia production is recognized as a viable method to support a sustainable artificial nitrogen cycle. Extensive research has been focused on enhancing the performance and selectivity of electrocatalysts for NO 3 - RR (nitrate reduction reaction). In this study, we show that modifying the surface oxygen species via thermal treatment and dispersant addition is an effective way to improve the NO 3 - RR performance of Cu 2 O/CF. Using advanced spectroscopic methods, we show that thermal treatment and dispersant addition can greatly boost the generation of oxygen vacancies and hydroxyl groups on the surface of Cu 2 O/CF. Electrocatalytic reaction rate experiment, in-situ FT-IR, DEMS analyses and DFT calculations further suggest that oxygen vacancies on the Cu 2 O/CF surface promote the adsorption and conversion of nitrate and its intermediate, nitrite. Meanwhile, hydroxyl groups promoted the selective hydrogenation of NO to NH 3 . Our findings highlight the essential role of surface oxygen species in NO 3 - RR and provide a foundation for designing advanced electrocatalysts through surface engineering approaches.
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Green Chemical Engineering
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2025
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IF 7.6
Jiankun Yu,Weixiao Sun,Kuan Huang,Jin Xu,Fuzeyu Zhong,Xiaohu Ge,Wenyao Chen,Gang Qian,Yueqiang Cao,Jianrong Zeng,Jianbo Ma,Xinggui Zhou,Xuezhi Duan,Jing Zhang,Lilong Jiang
Due to escalating carbon emissions, increasing attention is being focused on the synthesis of biomass-derived liquid fuels with a low CO 2 footprint. Currently, the dominant biobased liquid fuel in the diesel range is green diesel, produced via deoxygenation of non-edible natural/waste oils and their free fatty acid components into engine-compatible diesel-range alkanes. Industrially, sulfided NiMo or CoMo catalysts are typically used, leading to total hydrocarbon yields of 70-80 wt%. However, their inevitable sulfur leaching often contaminates the products and requires the addition of sulfur-containing agents. Here, we developed a highly selective sulfur-free Ni-Cu alloy catalyst by disentangling the electronic and size effects, to enable green diesel synthesis through the decarbonylation of palmitic acid—the most common fatty acid in these feedstocks. An unprecedented decarbonylation product (pentadecane) yield of 98% (on a molar basis) was achieved using a Ni-Cu alloy catalyst with a Ni/Cu ratio of 1:1 under mild reaction conditions (2 MPa H 2 , 250 °C). Minimal metal sintering or leaching was observed after multiple reuses. Kinetic studies show that incorporating Cu into Ni markedly reduces both the apparent activation energy and the reaction order for the conversion of palmitic acid. These results, combined with catalyst characterization, reveal that introducing Cu into Ni not only facilitates the adsorption and activation of the carboxylic hydroxyl group to promote the reductive deoxygenation of palmitic acid into aldehyde/alcohol intermediates—the slow step in decarbonylation—but also weakens the adsorption of C–C bonds on Ni by enhancing its electron density.
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