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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction 被引量:2
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作者 Kangwang Wang Zhuofeng Hu +8 位作者 Peifeng Yu Alina M.Balu Kuan Li Longfu Li Lingyong Zeng Chao Zhang Rafael Luque Kai Yan Huixia Luo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期68-84,共17页
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in... We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR. 展开更多
关键词 Quantum efficiency Electronic structure Steric interaction Bridging sites CO_(2)reduction
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Cu-Based Materials for Enhanced C_(2+) Product Selectivity in Photo-/Electro-Catalytic CO_(2) Reduction: Challenges and Prospects 被引量:1
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作者 Baker Rhimi Min Zhou +2 位作者 Zaoxue Yan Xiaoyan Cai Zhifeng Jiang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期25-66,共42页
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca... Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future. 展开更多
关键词 Photocatalytic CO_(2)reduction Cu-based materials Electrocatalytic CO_(2)reduction
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The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)for stable photocatalytic CO_(2)reduction 被引量:1
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作者 Yaqing Zhi Haoning Mao +5 位作者 Guangxing Yang Qiao Zhang Zhiting Liu Yonghai Cao Siyuan Yang Feng Peng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期104-112,共9页
Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)... Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future. 展开更多
关键词 CO_(2)photocatalytic reduction PHOTOCATALYSIS Basic copper carbonate SELF-RECONSTRUCTION PHOTOCATALYST
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Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst 被引量:1
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作者 Yingshi Su Yonghui Cheng +6 位作者 Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期543-551,I0012,共10页
Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Here... Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Herein,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance. 展开更多
关键词 Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product
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Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation 被引量:1
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作者 Qianying Lin Jiwu Zhao +8 位作者 Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期255-266,共12页
Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrat... Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic structure.It exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity.Specifically,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) pathway.This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts. 展开更多
关键词 artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC
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Electrocatalytic CO_(2)reduction to syngas
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作者 Bing Chang Zhaojun Min +4 位作者 Ning Liu Nan Wang Maohong Fan Jing Fan Jianji Wang 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第7期1085-1100,共16页
While carbon dioxide(CO_(2))is a major greenhouse gas,it is also an important C1 resource.In the trend of energy conservation and emission reduction,electrocatalytic reduction has become a very promising strategy for ... While carbon dioxide(CO_(2))is a major greenhouse gas,it is also an important C1 resource.In the trend of energy conservation and emission reduction,electrocatalytic reduction has become a very promising strategy for CO_(2)utilization because it can convert CO_(2)directly to high-valued chemicals and fuels under mild conditions.In particular,the product CO and by-product H_(2)can be combined into syngas by an electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in an aqueous medium.Different molar ratios of CO and H_(2)may be used to produce essential bulk chemicals or liquid fuels such as methanol,alkanes,and olefins through thermochemical catalysis,Fischer-Tropsch synthesis,microbial fermentation,and other techniques.This work discusses the latest strategies in controlling the molar ratio of CO/H_(2)and improving the yield of CO_(2)RR-to-syngas.The challenges of electrocatalytic syngas production are analyzed from an industrial application perspective,and the possible measures to overcome them are proposed in terms of new catalyst design,electrolyte innovation,flow reactor optimization,anodic reaction coupling,and operando technique application. 展开更多
关键词 ELECTROCATALYSIS CO_(2)reduction SYNGAS Electrolyte ELECTROLYZER
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Single-atom modified graphene cocatalyst for enhanced photocatalytic CO_(2) reduction on halide perovskite
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作者 Hui Fu Jin Tian +5 位作者 Qianqian Zhang Zhaoke Zheng Hefeng Cheng Yuanyuan Liu Baibiao Huang Peng Wang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期143-151,共9页
Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2) reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.Howe... Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2) reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.However,photoreduction of CO_(2) by MHP remains a challenge because of the slow charge separation and transfer.Herein,a cobalt single-atom modified nitrogen-doped graphene(Co-NG)cocatalyst is prepared for enhanced photocatalytic CO_(2) reduction of bismuth-based MHP Cs_(3)Bi_(2)Br_(9).The optimal Cs_(3)Bi_(2)Br_(9)/Co-NG composite exhibits the CO production rate of 123.16μmol g^(-1)h^(-1),which is 17.3 times higher than that of Cs_(3)Bi_(2)Br_(9).Moreover,the Cs_(3)Bi_(2)Br_(9)/Co-NG composite photocatalyst exhibits nearly 100% CO selectivity as well as impressive long-term stability.Charge carrier dynamic characterizations such as Kelvin probe force microscopy(KPFM),single-particle PL microscope and transient absorption(TA)spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance.The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement.In addition,in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers,demonstrating that the introduction of Co-NG promotes the formation of ^(*)COOH intermediate,providing sufficient evidence for the highly selective generation of CO.This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO_(2) reduction and is expected to shed light on other photocatalytic applications. 展开更多
关键词 Bismuth-based perovskite Photocatalysis CO_(2) reduction Single-atom cocatalyst Charge separation
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Modified TiO_(2)/In_(2)O_(3) heterojunction with efficient charge separation for visible-light-driven photocatalytic CO_(2) reduction to C_(2) product
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作者 Mengfang Liang Xiaodong Shao +8 位作者 Ji Yoon Choi Young Dok Kim Trang Thu Tran Jeongyong Kim Yosep Hwang Min Gyu Kim Yunhee Cho Sophia Akhtar Hyoyoung Lee 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期714-720,共7页
Utilizing sunlight to convert CO_(2) into chemical fuels could address the greenhouse effect and fossil fuel crisis,Heterojunction structure catalysts with oxygen vacancy are attractive in the field of photocatalytic ... Utilizing sunlight to convert CO_(2) into chemical fuels could address the greenhouse effect and fossil fuel crisis,Heterojunction structure catalysts with oxygen vacancy are attractive in the field of photocatalytic CO_(2) conversion.Herein,a modified TiO_(2)/In_(2)O_(3)(R-P2 5/In_(2)O_(3-x)) type Ⅱ heterojunction composite with oxygen vacancies is designed for photocatalytic CO_(2) reduction,which exhibits excellent CO_(2) reduction activity,with a C_(2) selectivity of 56.66%(in terms of R_(electron)).In situ Fourier-transform infrared spectroscopy(DRIFTS) and time-resolved photoluminescence(TR-PL) spectroscopy are used to reveal the intermediate formation of the photocatalytic mechanism and photogenerated electron lifetime,respectively.The experimental characterizations reveal that the R-P25/In_(2)O_(3-x) composite shows a remarkable behavior for coupling C-C bonds.Besides,efficient charge separation contributes to the improved CO_(2) conversion performance of photocatalysts.This work introduces a type Ⅱ heterojunction composite photocatalyst,which promotes understanding the CO_(2) reduction mechanisms on heterojunction composites and is valuable for the development of photocatalysts. 展开更多
关键词 HETEROJUNCTION Oxygen vacancy Photocatalytic CO_(2)reduction C_(2)product Charge separation
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Ligand modulation of active center to promote lead-free Cs_(2)AgInCl_(6)photocatalytic CO_(2)reduction
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作者 Baofei Sun Wei Chen +10 位作者 Yanyi Huang Daofu Wu Heng Luo Faguang Kuang Hongmei Ran Yichen Liu Liqin Gao Jinchen Zhou Bo Gao Qiang Huang Xiaosheng Tang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期660-669,I0015,共11页
Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand ... Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)reduction.The results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand modulation.Compared with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and CH_(4).The CO and CH_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts. 展开更多
关键词 Surface ligand Photocatalysis CO_(2)reduction Lead-free perovskite Reactive mechanism
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Regulating^(*)COOH intermediate via amino alkylation engineering for exceptionally effective photocatalytic CO_(2) reduction
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作者 Chengcheng Chen Qiaoyu Zhang +3 位作者 Fangting Liu Zhengguo Zhang Qiong Liu Xiaoming Fang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期282-291,共10页
Photocatalytic reduction of CO_(2) into fuel represents a promising approach for achieving carbon neutrality,while realizing high selectivity in this process is challenging due to uncontrollable reaction intermediate ... Photocatalytic reduction of CO_(2) into fuel represents a promising approach for achieving carbon neutrality,while realizing high selectivity in this process is challenging due to uncontrollable reaction intermediate and retarded desorption of target products.Engineering the interface microenvironment of catalysts has been proposed as a strategy to exert a significant influence on reaction outcomes,yet it remains a significant challenge.In this study,amino alkylation was successfully integrated into the melem unit of polymeric carbon nitrides(PCN),which could efficiently drive the photocatalytic CO_(2) reduction.Experimental characterization and theoretical calculations revealed that the introduction of amino alkylation lowers the energy barrier for CO_(2) reduction into^(*)COOH intermediate,transforming the adsorption of^(*)COOH intermediate from the endothermic to an exothermic process.Notably,the as-prepared materials demonstrated outstanding performance in photocatalytic CO_(2) reduction,yielding CO_(2)at a rate of 152.8μmol h^(-1) with a high selectivity of 95.4%and a quantum efficiency of 6.6%. 展开更多
关键词 Polymeric carbonnitride Regulate intermediate Photocatalytic CO_(2)reduction Amino alkylation ^(*)COOH adsorption
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Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction
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作者 Zhaoyong Jin Meiqi Yang +13 位作者 Yilong Dong Xingcheng Ma Ying Wang Jiandong Wu Jinchang Fan Dewen Wang Rongshen Xi Xiao Zhao Tianyi Xu Jingxiang Zhao Lei Zhang David J.Singh Weitao Zheng Xiaoqiang Cui 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期55-67,共13页
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,in... Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale. 展开更多
关键词 CO_(2)reduction reaction Atomic dispersed catalyst Hetero-diatomic pair Ad-desorption energy Linear scaling relation
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A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO_(2) reduction via dry-reforming of methane
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作者 Sheng-Yan Yin Ziyi Li +2 位作者 Yingcai Hu Xiao Luo Jishan Li 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第9期1407-1418,共12页
At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM) is quite promising and challenging.Herein,we developed a novel covalent organ... At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM) is quite promising and challenging.Herein,we developed a novel covalent organic porous polymer (TPE-COP) with rapid charge separation of the electron–hole pairs for DRM driven by visible light at room temperature,which can efficiently generate syngas (CO and H_(2)).Both electron donor (tris(4-aminophenyl)amine,TAPA) and acceptor (4,4',4'',4'''-((1 E,1'E,1''E,1'''E)-(ethene-1,1,2,2-tetrayltetrakis (benzene-4,1-diyl))tetrakis (ethene-2,1-diyl))tetrakis (1-(4-formylbenzyl)quinolin-1-ium),TPE-CHO) were existed in TPE-COP,in which the push–pull effect between them promoted the separation of photogenerated electron–hole,thus greatly improving the photocatalytic activity.Density functional theory (DFT) simulation results show that TPE-COP can form charge-separating species under light irradiation,leading to electrons accumulation in TPE-CHO unit and holes in TAPA,and thus efficiently initiating DRM.After 20 h illumination,the photocatalytic results show that the yields reach 1123.6 and 30.8μmol g^(-1)for CO and H_(2),respectively,which are significantly higher than those of TPE-CHO small molecules.This excellent result is mainly due to the increase of specific surface area,the enhancement of light absorption capacity,and the improvement of photoelectron-generating efficiency after the formation of COP.Overall,this work contributes to understanding the advantages of COP materials for photocatalysis and fundamentally pushes metal-free catalysts into the door of DRM field. 展开更多
关键词 METAL-FREE Photocatalytic CO_(2)reduction Covalent organic polymer Dry-reforming of methane Electron donor and acceptor
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Effects of surface chlorine atoms on charge distribution and reaction barriers for photocatalytic CO_(2)reduction
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作者 Wendong Zhang Wenjun Ma +6 位作者 Yuerui Ma Peng Chen Qingqing Ye Yi Wang Zhongwei Jiang Yingqing Ou Fan Dong 《Nano Materials Science》 EI CAS CSCD 2024年第2期235-243,共9页
Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are st... Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst. 展开更多
关键词 Surface chlorine atoms Charge distribution Reaction barriers Photocatalytic CO_(2)reduction Bi_(2)WO_(6)
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Research Progress in Photocatalytic CO_(2) Reduction with ZnIn_(2)S_(4)-Based Nanomaterials(Ⅰ)
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作者 CORDERO RODRIGUEZ Diana Vanessa TIAN Fengyu +1 位作者 XU Liwen YAN Xuemin 《化学与生物工程》 CAS 北大核心 2024年第11期1-8,共8页
Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2) reduction in recent years due to various advantages,includi... Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2) reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduced the types of ZISbased nanomaterials and their action mechanism in photocatalytic CO_(2) reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2) reduction. 展开更多
关键词 ZnIn_(2)S_(4) photocatalytic CO_(2)reduction HETEROSTRUCTURE charge separation
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Research Progress in Photocatalytic CO_(2)Reduction with ZnIn_(2)S_(4)-Based Nanomaterials(Ⅱ)
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作者 CORDERO RODR GUEZ Diana Vanessa +2 位作者 TIAN Fengyu XU Liwen YAN Xuemin 《化学与生物工程》 CAS 北大核心 2024年第12期1-8,共8页
Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2)reduction in recent years due to various advantages,includin... Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2)reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduce the types of ZIS-based nanomaterials and their action mechanism in photocatalytic CO_(2)reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2)reduction. 展开更多
关键词 ZnIn_(2)S_(4) photocatalytic CO_(2)reduction HETEROSTRUCTURE charge separation
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Catalytic reduction of SO_2 by CO over CeO_2-TiO_2 mixed oxides 被引量:5
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作者 张丽 秦毅红 +3 位作者 陈白珍 彭亚光 何汉兵 袁依 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2016年第11期2960-2965,共6页
The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. Acco... The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance. 展开更多
关键词 CeO2-TiO2 mixed oxides solid solution catalytic reduction carbon monoxide sulfur dioxide
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Resistance to SO_2 poisoning of V_2O_5/TiO_2-PILC catalyst for the selective catalytic reduction of NO by NH_3 被引量:4
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作者 臧思淼 张桂臻 +3 位作者 邱文革 宋丽云 张然 何洪 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第6期888-897,共10页
A titania pillared interlayered clay(Ti-PILC) supported vanadia catalyst(V2O5/TiO2-PILC) was prepared by wet impregnation for the selective catalytic reduction(SCR) of NO with ammonia. Compared to the traditiona... A titania pillared interlayered clay(Ti-PILC) supported vanadia catalyst(V2O5/TiO2-PILC) was prepared by wet impregnation for the selective catalytic reduction(SCR) of NO with ammonia. Compared to the traditional V2O5/TiO2 and V2O5-MoO3/TiO2 catalysts, the V2O5/TiO2-PILC catalyst exhibited a higher activity and better SO2 and H2O resistance in the NH3-SCR reaction. Characterization using TPD, in situ DRIFT and XPS showed that surface sulfate and/or sulfite species and ionic SO4^(2-)species were formed on the catalyst in the presence of SO2. The ionic SO4^(2-) species on the catalyst surface was one reason for deactivation of the catalyst in SCR. The formation of the ionic SO4^(2-) species was correlated with the amount of surface adsorbed oxygen species. Less adsorbed oxygen species gave less ionic SO4^(2-) species on the catalyst. 展开更多
关键词 Selective catalytic reduction TiO2-pillared clay Nitrogen oxide Vanadia catalyst In situ diffuse reflectance infrared Fourier transform spectroscopy
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Synthesis of novel MnO_x@TiO_2 core-shell nanorod catalyst for low-temperature NH_3-selective catalytic reduction of NOx with enhanced SO_2 tolerance 被引量:10
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作者 Zhongyi Sheng Dingren Ma +4 位作者 Danqing Yu Xiang Xiao Bingjie Huang Liu Yang Sheng Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第4期821-830,共10页
In this study,a MnOx@TiO2 core‐shell catalyst prepared by a two‐step method was used for the low‐temperature selective catalytic reduction of NOx with NH3.The catalyst exhibits high activity,high stability,and exce... In this study,a MnOx@TiO2 core‐shell catalyst prepared by a two‐step method was used for the low‐temperature selective catalytic reduction of NOx with NH3.The catalyst exhibits high activity,high stability,and excellent N2 selectivity.Furthermore,it displays better SO2 and H2O tolerance than its MnOx,TiO2,and MnOx/TiO2 counterparts.The prepared catalyst was characterized systematically by transmission electron microscopy,high‐resolution transmission electron microscopy,X‐ray diffraction,Raman,BET,X‐ray photoelectron spectroscopy,NH3 temperature‐programmed desorption and H2 temperature‐programmed reduction analyses.The optimized MnOx@TiO2 catalyst exhibits an obvious core‐shell structure,where the TiO2 shell is evenly distributed over the MnOx nanorod core.The catalyst also presents abundant mesopores,Lewis‐acid sites,and high redox capability,all of which enhance its catalytic performance.According to the XPS results,the decrease in the number of Mn4+active centers after SO2 poisoning is significantly lower in MnOx@TiO2 than in MnOx/TiO2.The core‐shell structure is hence able to protect the catalytic active sites from H2O and SO2 poisoning. 展开更多
关键词 Low-temperature selective catalytic reduction Core‐shell Nanorod SO2 resistance MNOX
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Supercritical water syntheses of transition metal-doped CeO_2 nano-catalysts for selective catalytic reduction of NO by CO:An in situ diffuse reflectance Fourier transform infrared spectroscopy study 被引量:12
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作者 Xiaoxia Dai Weiyu Jiang +4 位作者 Wanglong Wang Xiaole Weng Yuan Shang Yehui Xue Zhongbiao Wu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第4期728-735,共8页
In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice... In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice,forming solid solutions.The catalysts were then used for the selective catalytic reduction(SCR)of NO by CO.The Cu‐doped catalyst exhibited the highest SCR activity;it had a T50(i.e.,50%NO conversion)of only 83°C and a T90(i.e.,90%NO conversion)of 126°C.Such an activity was also higher than in many state‐of‐the‐art catalysts.In situ diffuse reflectance Fourier transform infrared spectroscopy suggested that the MOx‐CeO2 catalysts(M=Co and Fe)mainly followed an Eley‐Rideal reaction mechanism for CO‐SCR.In contrast,a Langmuir‐Hinshelwood SCR reaction mechanism occurred in CuO‐CeO2 owing to the presence of Cu+species,which ensured effective adsorption of CO.This explains why CuO‐CeO2 exhibited the highest activity with regard to the SCR of NO by CO. 展开更多
关键词 Supercritical water Nitrogen oxides CO Selective catalytic reduction Diffuse reflectance Fourier transform infrared spectroscopy CEO2
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Recent Advances in Interface Engineering for Electrocatalytic CO_(2) Reduction Reaction 被引量:13
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作者 Junjun Li Sulaiman Umar Abbas +2 位作者 Haiqing Wang Zhicheng Zhang Wenping Hu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2021年第12期499-533,共35页
Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically re... Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed. 展开更多
关键词 Interface engineering CO_(2)reduction reaction ELECTROCATALYSIS HETEROSTRUCTURE
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