Chinese Journal of Catalysis最新文献

{"title":"A chemoenzymatic cascade for sustainable production of chiral N-arylated aspartic acids from furfural and waste","authors":"Guang-Hui Lu,&nbsp;Jian Yu,&nbsp;Ning Li","doi":"10.1016/S1872-2067(24)60146-4","DOIUrl":"10.1016/S1872-2067(24)60146-4","url":null,"abstract":"<div><div>Both biomass valorization and waste upcycling are important routes to sustain the circular bioeconomy. In this work, we present a chemoenzymatic cascade for selective synthesis of chiral <em>N</em>-arylated aspartic acids from biomass-derived furfural and waste nitrophenols (NPs) by merging robust photo- and electrocatalysis with stereoselective biocatalysis. Concurrent photoelectrocatalytic oxidation of furfural into maleic acid (MA) and fumaric acid (FA) was significantly enhanced by combining catalyst and reaction engineering strategies including identification of a powerful photocatalyst meso-tetra(4-carboxyphenyl)porphyrin, continuous flow technique, enhancing dissolved O₂ and paired electrosynthesis. The overall space-time yield (STY) approached 2.8 g L⁻¹ h⁻¹ in a fed-batch process, with the product titer of 28.3 g L⁻¹. Besides, photoelectrosynthesis of MA/FA was effectively fueled by sunlight, with the STY of up to 3.6 g L⁻¹ h⁻¹. Both MA selectivity and yield could be facilely improved to around 89% by reducing the buffer concentrations. Paired electrosynthesis strategy not only resulted in greatly improved MA production at the anode, but also enabled NPs upcycling into value-added aminophenols (APs) at the cathode. The products formed in the two electrode chambers were converted into <em>N</em>-arylated (<em>S</em>)-aspartic acids by a bienzymatic cascade. This work presents a multicatalytic approach for integrating selective biomass valorization and waste upcycling towards sustainable manufacture.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 102-111"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143100114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Site requirements of supported W2C nanocatalysts for efficient hydrodeoxygenation of m-cresol to aromatics","authors":"Yanling Yang ,&nbsp;Peijie Han ,&nbsp;Yuanbao Zhang ,&nbsp;Jingdong Lin ,&nbsp;Shaolong Wan ,&nbsp;Yong Wang ,&nbsp;Haichao Liu ,&nbsp;Shuai Wang","doi":"10.1016/S1872-2067(24)60138-5","DOIUrl":"10.1016/S1872-2067(24)60138-5","url":null,"abstract":"<div><div>Selective hydrodeoxygenation of lignin derivatives into aromatic compounds is a promising route for the upgrading of lignin feedstocks. Metal carbide catalysts have exhibited excellent selectivity in hydrodeoxygenation reactions, while their structure-activity relationship is still in ambiguity. Herein, a liquid-phase atomic layer deposition method was employed to synthesize W₂C/SiO₂ catalysts with uniform and size-controllable W₂C nanoparticles. For gas-phase hydrodeoxygenation of lignin-derived <em>m</em>-cresol at 350 °C, these W₂C/SiO₂ catalysts showed superior toluene selectivities (&gt;95%) regardless of the W₂C particle size. An optimal W₂C particle size of ~7 nm was obtained for achieving the highest W₂C-based hydrodeoxygenation rate. In contrast, the turnover rate per surface W site increased almost monotonously as the W₂C particle size increased within 0.7‒15 nm, attributable to high-index planes appeared on the larger W₂C nanoparticles. Kinetic effects of <em>m</em>-cresol and H₂, taken together with temperature-programmed desorption of probe molecules and theoretical treatments, further indicate that the W₂C surface is nearly saturated by adsorbed <em>m</em>-cresol or its derivates under the reaction condition and the H-addition of the C₇H₇* intermediate to form toluene, instead of the initial C-O cleavage in <em>m</em>-cresol, acts as the rate-determining step. A side-by-side comparison between W₂C(102) and W₂C(001) catalyst surfaces in theoretical simulations of <em>m</em>-cresol hydrodeoxygenation verifies that high-index planes can stabilize kinetically-relevant transition states more effectively than the low-index ones, as a result of more available less-coordinated active sites on the former. The above findings bring new mechanistic insights into the site requirements of supported W₂C nanocatalysts, distinct from those metal-catalyzed hydrodeoxygenation of oxygenates.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 91-101"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient low-temp direct air capture methods","authors":"Hao Zhang,&nbsp;Yong Wang","doi":"10.1016/S1872-2067(24)60169-5","DOIUrl":"10.1016/S1872-2067(24)60169-5","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 1-3"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Silicalite-1 zeolite nanosheets with rich H-bonded silanols for boosting vapor-phase Beckmann rearrangement: One-pot synthesis and theoretical investigation","authors":"Tianming Zai ,&nbsp;Wei Chen ,&nbsp;Jiamin Yuan ,&nbsp;Ye Ma ,&nbsp;Qinming Wu ,&nbsp;Xianfeng Yi ,&nbsp;Zhiqiang Liu ,&nbsp;Xiangju Meng ,&nbsp;Weiliao Liu ,&nbsp;Na Sheng ,&nbsp;Han Wang ,&nbsp;Anmin Zheng ,&nbsp;Feng-Shou Xiao","doi":"10.1016/S1872-2067(24)60160-9","DOIUrl":"10.1016/S1872-2067(24)60160-9","url":null,"abstract":"<div><div>Design and preparation of highly efficient zeolite catalysts for gas-phase Beckmann rearrangement of cyclohexanone oxime to caprolactam are attractive but still challenging. Herein, we show a one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols. The key to this success is the use of urea in the synthetic system. Catalytic tests of cyclohexanone oxime gas-phase Beckmann rearrangement show that the silicalite-1 zeolite nanosheets with H-bonded silanols exhibit higher selectivity for caprolactam and longer reaction lifetime than those of the conventional silicalite-1 zeolite. Theoretical simulations reveal that the ammonium decomposed by urea is a critical additive for the formation of H-bond silanols. Obviously, one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols plus excellent catalytic performance in the Beckmann rearrangement offer a new opportunity for development of highly efficient zeolites for catalytic applications in the future.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 82-90"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172202","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Selective photooxidation of methane to C1 oxygenates by constructing heterojunction photocatalyst with mild oxidation ability","authors":"Hantao Gong ,&nbsp;Caihao Deng ,&nbsp;Peipei He ,&nbsp;Mingjie Liu ,&nbsp;Yiliang Cai ,&nbsp;Yiwen Yang ,&nbsp;Qiwei Yang ,&nbsp;Zongbi Bao ,&nbsp;Qilong Ren ,&nbsp;Siyu Yao ,&nbsp;Zhiguo Zhang","doi":"10.1016/S1872-2067(24)60136-1","DOIUrl":"10.1016/S1872-2067(24)60136-1","url":null,"abstract":"<div><div>Selective photocatalytic aerobic oxidation of methane to value-added chemicals offers a promising pathway for sustainable chemical industry, yet remains a huge challenge owing to the consecutive overoxidation of primary products. Here, a type II heterojunction were constructed in Ag-AgBr/ZnO to reduce the oxidation potential of stimulated holes and prevent the undesirable CH₄ overoxidation side reactions. For photocatalytic oxidation of methane under ambient temperature, the products yield of 1499.6 μmol g_cat⁻¹ h⁻¹ with a primary products selectivity of 77.9% was achieved over Ag-AgBr/ZnO, which demonstrate remarkable improvement compared to Ag/ZnO (1089.9 μmol g_cat⁻¹ h⁻¹, 40.1%). The superior activity and selectivity result from the promoted charge separation and the redox potential matching with methane activation after introducing AgBr species. Mechanism investigation elucidated that the photo-generated holes transferred from the valence band of ZnO to that of AgBr, which prevent H₂O oxidation and enhance the selective generation of •OOH radical.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 61-70"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Non-derivatized metal-organic framework nanosheets for water electrolysis: Fundamentals, regulation strategies and recent advances","authors":"Yingjie Guo ,&nbsp;Shilong Li ,&nbsp;Wasihun Abebe ,&nbsp;Jingyang Wang ,&nbsp;Lei Shi ,&nbsp;Di Liu ,&nbsp;Shenlong Zhao","doi":"10.1016/S1872-2067(24)60153-1","DOIUrl":"10.1016/S1872-2067(24)60153-1","url":null,"abstract":"<div><div>Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen. Currently, noble metal (e.g. Iridium, Ruthenium, Platinum)-based catalysts are most widely used for water splitting electrolysis. However, noble metal-based catalysts often suffer from multiple disadvantages, including high cost, low selectivity and poor durability. The emergence of metal-organic framework nanosheets (MOFNSs) attracts significant attention due to their unique advantages. Here, a concise, yet comprehensive and critical, review of recent advances in the field of MOFNSs is provided. This review explains the fundamental oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed. Moreover, it discusses efficient design strategies and the brief research advances of MOFNSs in HER, OER, and bifunctional electrocatalysis, along with some challenges and opportunities.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 21-53"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual-metal synergy unlocking ROS-free catalysis for rapid aerobic oxidation of 5-hydroxymethylfurfural at room temperature","authors":"Meiyun Zhang ,&nbsp;Penghua Che ,&nbsp;Hong Ma ,&nbsp;Xin Liu ,&nbsp;Shujing Zhang ,&nbsp;Yang Luo ,&nbsp;Jie Xu","doi":"10.1016/S1872-2067(24)60151-8","DOIUrl":"10.1016/S1872-2067(24)60151-8","url":null,"abstract":"<div><div>Clean catalytic oxidation has a broad prospect in the modern chemical engineering and energy chemistry fields. However, unexpected over-oxidation and disruptive degradation are frequently induced by excessive reactive oxygen species (ROS). Herein, we reported a new ROS-free approach to effectively drive O₂ to be activated into highly reactive surface peroxo species through enzyme-mimicking mechanism. Benefiting from the dual-metal synergy effect between Cu and Co active sites, ROS (H₂O₂ and OH^•) is generated <em>in situ</em> while further scavenged completely into surface peroxo species, which gives rise to very high selectivity and extremely high carbon balance. For example, the CuCo/N-C catalyst affords &gt;99.8% conversion and 94.5% selectivity to 2,5-furanedicarboxylic acid at 25 °C for 6 h in the aerobic oxidation of biomass platform 5-hydroxymethylfurfural. Moreover, it achieved exceptional performance in the oxidation of a variety of hydroxyl compounds to organic acids with high yields (89.9%–99.5%) at a mild temperature (25–40 °C). This exploration introduces an innovative clue for emulating enzyme catalysts, thereby enriching our comprehension and advancement of biologically inspired catalytic oxidations.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 144-156"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Artificial metalloenzymes enabled by combining proteins with hemin via protein refolding","authors":"Jingping Ouyang ,&nbsp;Zhenfang Zhang ,&nbsp;René Hübner ,&nbsp;Henrik Karring ,&nbsp;Changzhu Wu","doi":"10.1016/S1872-2067(24)60150-6","DOIUrl":"10.1016/S1872-2067(24)60150-6","url":null,"abstract":"<div><div>In this study, we unveil a conceptual technology for fabricating artificial metalloenzymes (ArMs) by deeply integrating hemin into protein scaffolds <em>via</em> a protein refolding process, a method that transcends the conventional scope of surface-level modifications. Our approach involves denaturing proteins, such as benzaldehyde lyase, green fluorescent protein, and <em>Candida antarctica</em> lipase B, to expose extensive reactive amino acid residues, which are then intricately linked with hemin using orthogonal click reactions, followed by protein refolding. This process not only retains the proteins’ structural integrity but expands proteins’ functionality. The most notable outcome of this methodology is the hemin@BAL variant, which demonstrated a remarkable 83.7% conversion rate in cyclopropanation reactions, far surpassing the capabilities of traditional hemin-based catalysis in water. This success highlights the significant role of protein structure in the ArMs’ activity and marks a substantial leap forward in chemical modification of proteins. Our findings suggest vast potentials of protein refolding approaches for ArMs across various catalytic applications, paving the way for future advancements in synthetic biology and synthetic chemistry.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 157-165"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Edge effect-enhanced CO2 adsorption and photo-reduction over g-C3N4 nanosheet","authors":"Xuedong Jing ,&nbsp;Xiaoyun Mi ,&nbsp;Wei Lu ,&nbsp;Na Lu ,&nbsp;Shiwen Du ,&nbsp;Guodong Wang ,&nbsp;Zhenyi Zhang","doi":"10.1016/S1872-2067(24)60141-5","DOIUrl":"10.1016/S1872-2067(24)60141-5","url":null,"abstract":"<div><div>Effective CO₂ adsorption and fast electron injection are two crucial processes of photocatalysts for achieving high-efficiency CO₂ photo-reduction. However, simultaneously enhancing these processes within a single photocatalyst remains a challenging task. Herein, we propose an intriguing edge effect based on the intrinsic atomic structure of g-C₃N₄ nanosheets (NSs) to enhance their CO₂ adsorption and facilitate the transfer of photo-generated electrons to the adsorbed CO₂. By cutting large pieces of g-C₃N₄ NSs into smaller fragments, the exposure of amino groups at the edges of its repeating tri-s-triazine units can be significantly increased. These edge-exposed amino groups serve as active sites for enhancing the CO₂ capture capacity of g-C₃N₄ NSs. As we decrease the lateral size of g-C₃N₄ NSs from tens of micrometers to hundreds of nanometers, their CO₂ adsorption capacity increases from 4.74 to 8.56 cm³ g⁻¹. Reducing the size of g-C₃N₄ NSs also facilitates the transfer of photo-generated electrons to the edge-adsorbed CO₂. Thus, our optimized g-C₃N₄ NSs with the edge effect exhibits a 37-fold enhancement in activity for CO₂ photo-reduction compared to normal g-C₃N₄ NSs under simulated sunlight irradiation. Notably, by introducing Pt cocatalysts, we can control product selectivity from 85.9% CO to 97.9% CH₄.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 112-123"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"LSPR-assisted W18O49/ZnO S-scheme heterojunction for efficient photocatalytic CO2 N-formylation of aniline","authors":"Jiafa Chen ,&nbsp;Peng Bai ,&nbsp;Shibo Yuan ,&nbsp;Yi He ,&nbsp;Zifan Niu ,&nbsp;Yicheng Zhao ,&nbsp;Yongdan Li","doi":"10.1016/S1872-2067(24)60149-X","DOIUrl":"10.1016/S1872-2067(24)60149-X","url":null,"abstract":"<div><div>Designing highly efficient photocatalyst for the valorization of CO₂ is an ideal strategy to reduce greenhouse gas emissions and utilize solar energy. In this study, a S-scheme heterojunction photocatalyst is fabricated by solvothermal impregnation of ZnO on W₁₈O₄₉ for photocatalytic CO₂ <em>N</em>-formylation of aniline. The localized surface plasmon resonance effect of W₁₈O₄₉ improves the absorption capacity for long-wave light significantly, and the hot electrons generated in W₁₈O₄₉ with a high energy can migrate to the conduction band of ZnO and thus enhance the photocatalytic reduction ability. Meanwhile, the S-scheme heterojunction facilitates the separation of photoinduced charge carriers and preserves the redox ability of W₁₈O₄₉/ZnO composite photocatalyst. The conversion of aniline reaches 99.1% after 5 h reaction under visible light irradiation at room temperature with an <em>N</em>-formylaniline selectivity of 100%. A possible photocatalytic reaction mechanism is proposed. This study paves a promising way for the design of highly efficient photocatalyst and the sustainable utilization of CO₂.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 124-134"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}