C2 Products Research Articles

TM and P dual sites on polymeric carbon nitride enable highly selective CO reduction to C2 products with low potentials: A theoretical perspective.

The CO reduction reaction (CORR) for the production of high-value-added multi-carbon (C2+) products is currently being actively investigated, where searching for high-efficiency catalysts with moderate CO intermediate binding strength and low kinetic barrier for C-C coupling poses a significant challenge. In this study, we employed density functional theory computations to design four synergistic coupling dual sites catalysts for CORR to C2 products, namely, TM-P@melon, by co-doping transition metals (TM = Mn, Fe, Co, and Ni) and phosphorus (P) into the polymeric carbon nitride (i.e., melon-CN). Mn-P@melon and Ni-P@melon exhibit higher selectivity toward C2H5OH and C2H6, respectively, with limiting potentials (C-C coupling kinetic energy barriers) of -0.43V (0.52eV) and -0.17V (0.26eV), respectively. The introduction of TM and P atoms not only narrows the band gap of melon-CN but also favors the coupling of CO and *CHO, providing an active site for C-C coupling, thus facilitating the catalytic reaction. Our work provides rational insights for the design of stable, low-cost, and efficient CORR dual sites catalysts that facilitate the sustainable production of high-value C2 chemicals and fuels.

Influence of Dopants on Pt/Al2O3-Based Monolithic Catalysts for Autothermal Oxidative Coupling of Methane

Autothermal oxidative coupling of methane (OCM) is a highly attractive approach for methane utilization. If platinum-based catalysts are operated in short-contact-time reactors with high space velocities, high methane conversion can be achieved. Using a 1 wt.% Pt/Al2O3 catalyst as a benchmark, the present study elucidates how different dopants, namely Ni, Sn, and V2O5, affect the OCM reaction. Kinetic catalyst tests reveal that acetylene (C2H2) is the predominant C2 product, irrespective of the catalyst formulation or operation conditions. Furthermore, the use of bimetallic catalysts allows either for the maintenance or even the improvement of the C2 selectivity during OCM, which is attributed to synergistic effects that occur when expensive Pt is partially replaced by cheaper dopants. In particular, the 1 wt.% Pt/Al2O3 reference catalyst yielded a maximum C2 selectivity of 8.2%, whereas the best-performing doped sample 0.25 wt.% Pt 0.75 wt.% V2O5/Al2O3 yielded a total C2 selectivity of 11.3%.

Bioconversion of C1 and C2 artificial photosynthesis products into high-value bioproducts by mixotrophic microalgae Chlorella pyrenoidosa

This study investigated the use of C1 and C2 products synthesized through artificial photosynthesis to enhance the growth and synthesis of pigments, starches, and lipids of Chlorella pyrenoidosa. Compared with the control group, potassium acetate and ethanol significantly promoted the growth of microalgae, while methanol and potassium formate showed certain inhibitory effects on the growth of microalgae, indicating that C2 products were more conducive to the growth of microalgae. It is worth noting that the ability of microalgae to utilize potassium formate after domestication was significantly enhanced, indicating that domestication treatment of microalgae is an effective means to improve the utilization rate of C1 products. Both C1 and C2 products significantly promoted the accumulation of lipid and starch in microalgae cells, and C2 products significantly increased the lipid and starch yield of microalgae, with potassium acetate being the most effective. Under the treatment of 5 g/L potassium acetate, biomass productivity of C. pyrenoidosa reached 0.28 g/L d−1, while starch and lipid yield reached 17.2 mg/L d−1 and 25.2 mg/L d−1, respectively. Transcriptomic analysis revealed significant upregulation of genes involved in photosynthesis, energy metabolism and other elated pathways under the influence of different organics. Furthermore, the addition of potassium acetate and formate reduced the dependency of microalgae on photosynthesis, while ethanol and potassium acetate significantly accelerated the energy metabolism of microalgae, establishing the basis for microalgae growth and biomass production. In conclusion, potassium acetate was found to be a relatively suitable product of artificial photosynthesis for enhancing the production of high-value bioproducts by mixotrophic microalgae, and when C1 products were used for microalgae culture, pretreatment such as microalgae domestication was particularly important

Highly Active Photoreduction of Atmospheric‐Concentration CO2 into CH3COOH over Palladium Particles on Nb2O5 Nanosheets

AbstractThe endeavor to drive CO2 photoreduction towards the synthesis of C2 products is largely thwarted by the colossal energy hurdle inherent in C−C coupling. Herein, we load active metal particles on metal oxide nanosheets to build the dual metal pair sites for steering C−C coupling to form C2 products. Taking Pd particles anchored on the Nb2O5 nanosheets as an example, the high‐angle annular dark‐field image and X‐ray photoelectron spectroscopy demonstrate the presence of Pd−Nb metal pair sites on the Pd‐Nb2O5 nanosheets. Density functional theory calculations reveal these sites exhibit a low reaction energy barrier of only 1.02 eV for C−C coupling, implying that the introduction of Pd particles effectively tailors the reaction step to form C2 products. Therefore, the Pd‐Nb2O5 nanosheets achieve a CH3COOH evolution rate of 13.5 μmol g−1 h−1 in photoreduction of atmospheric‐concentration CO2, outshining all other single photocatalysts reported to date under analogous conditions.

Enhanced Stability and Selectivity in Pt@MFI Catalysts for n-Butane Dehydrogenation: The Crucial Role of Sn Promoter

The dehydrogenation of n-butane to butenes is a crucial process for producing valuable petrochemical intermediates. This study explores the role of oxyphilic metal promoters (Sn, Zn, and Ga) in enhancing the performance and stability of Pt@MFI catalysts for n-butane dehydrogenation. The presence of Sn in the catalyst inhibits the agglomeration of Pt clusters, maintaining their subnanometric particle size. PtSn@MFI exhibits superior stability and selectivity for butenes while suppressing cracking reactions, with selectivity for C1–C3 products as low as 2.1% at 550 °C compared to over 30.5% for Pt@MFI. Using a combination of high-angle annular dark-field scanning transmission electron microscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, and Raman spectroscopy, we examined the structural and electronic properties of the catalysts. Our findings reveal that Zn tends to consume hydroxyl groups and substitute framework sites, and Ga induces more defective sites in the zeolite structure. In contrast, the interaction between SnOx and the zeolite framework does not depend on reactions with hydroxyl groups. The incorporation of Sn significantly prevents Pt particle agglomeration, maintaining smaller Pt particle sizes and reducing coke formation compared to Zn and Ga promoters. Theoretical calculations showed that Sn increases the positive charge on Pt clusters, enhancing their interaction with the zeolite framework and reducing sintering, albeit with a slight increase in the energy barrier for C-H activation. These results underscore the dual benefits of Sn as a promoter, offering enhanced structural stability and reduced coke formation, thus paving the way for the rational design of more effective and durable catalysts for alkane dehydrogenation and other high-value chemical processes.

Selective electroreduction of CO2 to value-added C1 and C2 products using MOF and COF-based catalysts

Selective electroreduction of CO2 to value-added C1 and C2 products using MOF and COF-based catalysts

Rationale and design of the SHASTA-3 and SHASTA-4 studies: randomized, double-blind, placebo-controlled, phase 3 studies of plozasiran in patients with severe hypertriglyceridemia

Abstract Severe hypertriglyceridemia (sHTG) confers an increased risk of atherosclerotic cardiovascular disease (ASCVD) and acute pancreatitis (AP). sHTG-associated AP is a substantial source of morbidity, mortality, reduced quality of life and financial burden to health care systems. Currently available therapeutic approaches for sHTG are often insufficient to reduce triglyceride (TG) levels and prevent AP. Plozasiran, an investigational siRNA therapeutic, inhibits hepatic production of apolipoprotein C3 (APOC3), a key regulator of lipoprotein lipase-mediated TG metabolism and clearance. In a phase 2 study of sHTG patients [TG ≥500 mg/dL (≥5.65 mmol/L)], plozasiran demonstrated durable reductions in TG levels of up to -80%, 12 weeks after the last dose, and decreased TG below 500 mg/dL (5.65 mmol/L), a threshold of increased risk for AP in most participants. The SHASTA-3 and SHASTA-4 trials will evaluate safety and efficacy of plozasiran, including AP rates, in patients with sHTG. SHASTA-3 and SHASTA-4 are phase 3, randomized, double-blind, placebo-controlled, multi-center trials. Key inclusion criteria are prior sHTG and fasting TG ≥500 mg/dL (≥5.65 mmol/L), at screening. Key exclusion criteria include use of any hepatocyte targeted siRNA treatments that target lipids and/or TGs within 1 year (except inclisiran at least 4 weeks prior to enrollment), siRNA or ASO within 60 days, known FCS diagnosis, and AP within 4 weeks of screening. 700 adults with sHTG will be enrolled in these two trials in several sites across multiple countries. Patients will be randomized 2:1 to receive 4 quarterly subcutaneous injections of plozasiran 25 mg or matching placebo over a 1-year double-blinded period, followed by post-treatment evaluation or entry into the open-label extension study. The randomization will be stratified based on TG levels (≥880 mg/dL vs <880 mg/dL [≥ vs <10 mmol/L]) and prior history of AP, within 5 years of screening. The primary efficacy endpoint of the studies is placebo-adjusted percent change in fasting TG from baseline to month 12 with plozasiran. Secondary endpoints include percent change in fasting TG from baseline to month 10 compared to placebo, percent of patients achieving fasting TGs of <500 mg/dL (<5.65 mmol/L) and TGs of <150 mg/dL (<1.69 mmol/L) at month 10 and 12 compared to placebo, and event rate of adjudicated abdominal clinical events including ER visits and hospitalization for abdominal pain attributed to HTG and events of documented pancreatitis. The effect of plozasiran on other lipids and lipoproteins, inflammatory biomarkers, and liver fat content using magnetic resonance imaging-proton density fat fraction will be assessed. Adjudicated major adverse cardiovascular event rates, safety and tolerability will be assessed. SHASTA-3 and SHASTA-4 are designed to determine whether the quarterly-dosed APOC3 siRNA plozasiran, added to standard of care, safely reduces TG levels and the rate of AP in patients with sHTG.

Nickel-Doped Facet-Selective Copper Nanowires for Activating CO-to-Ethanol Electrosynthesis.

Ethanol isa promising energy vector for closing the anthropogenic carbon cycle through reversible electrochemical redox. Currently, ethanol electrosynthesissuffers from low product selectivity due to the competitive advantage of ethylene in CO2/CO electroreduction. Here, a facet-selective metal-doping strategy is reported, tuning the reaction kinetics of CO reduction paths and thus enhancing the ethanol selectivity. The theoretical calculations reveal that nickel (Ni)doped Cu(100) surface facilitates water dissociation to form adsorbed hydrogen, which promotesselective electrochemical hydrogenation of a key C2 intermediate (*CHCOH) toward ethanol path over ethylene path. Experimentally, a solution-phase synthesis of a Ni-doped {100}-dominated Copper nanowires (Cu NWs) catalyst is reported, enabling an ethanol Faradaic efficiency of 56% and a selectivity ratio of ethanol to ethylene of 2.7, which are ≈4 and 15 times larger than those of undoped Cu NWs, respectively. The operando spectroscopic characterizationsconfirm that Ni-doping in Cu NWs can alter the interfacial water activity and thus regulate the C2 product selectivity. With further electrode engineering, a membrane electrode assembly electrolyzer using Ni-doped Cu NWs catalysts demonstrates an ethanol Faradaic efficiency over 50% at 300mA cm-2 with a full cell voltage of ≈2.7V and operates stably for over 300 h.

Efficient CO2 Reduction Reaction on Cu-Decorated Biphenylene.

Developing efficient electrocatalysts for CO2 reduction into value-added products is crucial for a green economy. Inspired by the recent experimental synthesis of biphenylene (BPH) and the excellent catalytic activity of copper dispersed on two-dimensional (2D) materials, we chose to systematically investigate the pristine, defective, and Cu-decorated BPH for the electrocatalytic CO2 reduction to value-added hydrocarbons. It is observed that the CO2 molecules bind weakly to the pristine BPH, indicating their chemical inertness. Carbon single-vacancy defects facilitate CO2 adsorption with a strong binding energy (Eb) of -3.23 eV, detrimental to the CO2 reduction reaction (CRR) mechanism. We have further investigated the binding energy and kinetic stability of Cu-decorated BPH as a single-atom-catalyst (SAC). The molecular dynamics simulations confirm the kinetic stability, revealing that the Cu-atom avoids agglomeration under low metal dispersal conditions. The CO2 molecule gets adsorbed horizontally on the Cu-BPH surface with a ΔEb of -0.52 eV. The CRR mechanism is investigated using two pathways beginning with two different initial states, formate (*OCOH) and carboxylic (*COOH). The formate pathway confirms the conversion of *OCOH to *HCOOH with the rate-limiting potential (UL) of 0.39 eV for the production of HCOOH, while for the carboxylic pathway, the conversion of *COH to *CHOH has a UL of 0.32 eV, eventually producing CH3OH. Our findings highlight the role of Cu-BPH as an efficient SAC for CO2 catalytic activity to C1 products, as compared to the state-of-the-art Cu, and holds promise as an electrocatalyst for CRR.

Unconventional Electrocatalytic CO Conversion to C2 Products on Single-Atomic Pd-Agn Sites.

The electrochemical reduction of CO or CO2 into C2+ products has mostly been focused on Cu-based catalysts. Although Ag has also been predicted as a possible catalyst for the CO-to-C2+ conversion from the thermodynamic point of view, however, due to its weak CO binding strength, CO rapidly desorbs from the Ag surface rather than participates in deep reduction. In this work, we demonstrate that single-atomic Pd sites doped in Ag lattice can tune the CO adsorption behavior and promote the deep reduction of CO toward C2 products. The monodispersed Pd-Agn sites enable the CO adsorption with both Pd-atop (PdL) and Pd-Ag bridge (PdAgB) configurations, which can increase the CO coverage and reduce the C-C coupling energy barrier. Under room temperature and ambient pressure, the Pd1Ag10 alloy catalyst exhibited a total CO-to-C2 Faradaic efficiency of ~37 % at -0.83 V, with appreciable current densities and electrochemical stability, thus featuring unconventional non-Cu electrocatalytic CO-to-C2 conversion capability.

Tailoring electrochemical CO2 reduction selectivity over CuSn by modulating surface oxidation state with infrared laser treatment

Infrared laser treatment was used to precisely modify the surface structure of CuSn electrodes, effectively fine-tuning the selectivity of reduction products. With increasing laser power, the metallic Cu and Sn surfaces became more oxidized, and the Sn/Cu composition ratio varied with depth and further changed post-EC reaction. The diversity of reduction products, including C1 (CO, CH4, and formate), C2 (C2H4, ethanol, acetate, acetaldehyde, and glycolaldehyde), and C3 (propanol and isopropanol) compounds, shifted towards a more selective production of C1 (CO and formate) products. These tailored behaviors are attributed to variations in interfacial electronic structures, oxidation states, composition ratios, and the interaction between CO2 and the density of states (Cu, O, and Sn) near the Fermi level. The laser treatment method enables precise tuning of electrode surfaces, modulation of reduction products, and enhancement of selectivity. Moreover, this technique presents a novel approach for electrode design in the field of CO2 reduction, offering new avenues for optimizing catalytic performance.

Understanding Selectivity in Product Distributions from Laser Ablation of Organic Liquids.

Pulsed laser ablation in organic solvents is widely used to produce oxide-free metal and metal carbide nanoparticles, often with carbon coatings resulting from laser-induced reactions in the organic solvent. To gain insight into how the molecular structure of the solvent affects these reaction pathways, this work investigates ablation of the C6H14 isomers n-hexane, 2-methylpentane, and 3-methylpentane through characterization of the gas and liquid products with mass spectrometry. Ablation of each C6H14 isomer produces a distinct distribution of product molecular weights and isomers. 2-methylpentane preferentially produces C3 and C9, whereas 3-methylpentane produces C2, C4, C8, and C10 products. These preferential product distributions, along with the lack of such selectivity in n-hexane, arise from differences in the most favorable C-C bond scission pathways in each C6H14 isomer. Moreover, the particular isomers of C8H18, C9H20, C10H22, and C12H26 produced by ablation of each C6H14 isomer indicate that the vast majority of reaction pathways involve addition reactions between a fragment radical and parent C6H14 or between two C6H14 molecules, without molecular rearrangement. This propensity toward direct addition suggests that the chemical reactions induced by ultrashort pulsed laser ablation proceed on faster time scales than those of radical rearrangements.

Radiation-Synthesized Metal-Organic Frameworks with Ligand-Induced Lewis Pairs for Selective CO2 Electroreduction.

The electrochemical activation of inert CO2 molecules through C─C coupling reactions under ambient conditions remains a significant challenge but holds great promise for sustainable development and the reduction of CO2 emission. Lewis pairs can capture and react with CO2, offering a novel strategy for the electrosynthesis of high-value-added C2 products. Herein, an electron-beam irradiation strategy is presented for rapidly synthesizing a metal-organic framework (MOF) with well-defined Lewis pairs (i.e., Cu- Npyridinic). The synthesized MOFs exhibit a total C2 product faradic efficiency of 70.0% at -0.88V versus RHE. In situ attenuated total reflection Fourier transform infrared and Raman spectra reveal that the electron-deficient Lewis acidic Cu sites and electron-rich Lewis basic pyridinic N sites in the ligand facilitate the targeted chemisorption, activation, and conversion of CO2 molecules. DFT calculations further elucidate the electronic interactions of key intermediates in the CO2 reduction reaction. The work not only advances Lewis pair-site MOFs as a new platform for CO2 electrochemical conversion, but also provides pioneering insights into the underlying mechanisms of electron-beam irradiated synthesis of advanced nanomaterials.

Improving Glycerol Electrooxidation Performance on Nanocubic PtCo Catalysts.

As glycerol (GLY) has emerged as a highly functional and cheap platform molecule and as an abundant biodiesel production byproduct, possible conversion methods have been investigated. One of the promising approaches is the glycerol electrooxidation (GEOR) on noble metal-based catalysts. Although noble metals, especially Pt, are generally very stable at different pH and highly selective toward three-carbon (C3) products, their electrocatalytic performance can be further improved by morphology tuning and alloying with non-noble metals like Co. In the present study, cubic PtxCo100-x (x = 100, 80, and 60) nanoparticles were investigated in an alkaline medium at 20 and 40 °C. The effect of the composition and reaction conditions on the selectivity of the GEOR toward C3 products like lactate and glycerate was studied, and the reaction mechanism was discussed. The highest mass activity was found for Pt80Co20, although when the specific activity, glycerol conversion, and GEOR selectivity were compared, Pt60Co40 was the superior catalyst overall. In general, all catalysts, even those that are Co-rich, exhibited a high C3 product selectivity up to 95% at 0.67 V vs RHE. The low applied potential of 0.67 V vs RHE at 40 °C facilitated lactate formation with selectivity up to 72%. At the same time, the glycerate formation with a selectivity of up to 40%, as well as C-C bond cleavage, was more favored at 0.87 V vs RHE.

Ag-Mediated Growth of Au/Ag-Cu Ternary Heterostructures for Selective Electrochemical CO2 Reduction.

Copper (Cu)-based nanocatalysts play crucial roles in the electrochemical CO2 reduction reaction (ECO2RR) for sustainable energy resources. Particularly, Cu-based nanostructures incorporating Au and Ag are promising, offering enhanced activity, selectivity, and stability. However, precise control over the structure and composition of heterostructures remains challenging, hindering the development of highly efficient catalysts. Herein, we present a silver (Ag) transition-layer-mediated approach to synthesize ternary heterostructures with two specific morphologies, namely, Au/Ag-Cu-side and Au/Ag-Cu-tip, which exhibit different Ag-Cu interface epitaxial patterns. The two heterostructures achieve high C2 product selectivity in ECO2RR. Especially, the Au/Ag-Cu-side structure achieves 50.3% C2 selectivity with 35.5% ethanol, while the tip structure shows higher ethylene selectivity. Our study reveals the impact of the Ag layer in directing deposition sites on heterostructure growth and further facilitating the design of multicomponent Cu-based catalysts with enhanced structural integrity and ECO2RR performance.

Cu−based bimetallic sites' p-d orbital hybridization promotes CO asymmetric coupling conversion to C2 products

Hampered by sluggish C−C coupling kinetics, the low selectivity and efficiency have limited industrial applications of CO2 reduction into valuable multi-carbon products. A direct coupling of CO molecules or their coupling after hydrogenation, followed by the final synthesis of C2 products, can help to overcome these limitations potentially. In this study, a detailed high-throughput screening of bimetallic site catalysts comprising copper (Cu) and 28 other metal (M) atoms was conducted. The metal atoms Cu and M were anchored on a carbon nanotube (CNT) with six nitrogen (N6) defects (CuMN6@CNT), which possesses effective dual active sites for C−C coupling. The calculated results demonstrate that the CuGaN6@CNT catalyst exhibited favorable selectivity, with low theoretical overpotentials of −0.23 and −0.34 eV for ethanol and ethylene, respectively, surpassing most reported catalysts. The synergistic effect of Ga and Cu sites, along with their p-d states hybridization, results in an enhancement of Cu's d state dispersion and energy barriers reduction for C−C coupling. Additionally, the strain effect of the substrate CNT exhibits a direct correlation with the catalytic performance of CuGaN6@CNT by adjusting the d-band center of the Cu site and p-band center of the Ga site. These findings provide a novel insights into the electrocatalytic reduction of CO into valuable C2 products using bimetallic single atom catalyst, offering significant guidance for future research endeavors in this field.

Dual Active Sites with Charge‐asymmetry in Organic Semiconductors Promoting C‐C Coupling for Highly Efficient CO2 Photoreduction to Ethanol

Selective CO2 photoreduction into high‐energy‐density and high‐value‐added C2 products is an ideal strategy to achieve carbon neutrality and energy shortage, but it is still highly challenging due to the large energy barrier of the C‐C coupling step and severe exciton annihilation in photocatalysts. Herein, strong and localized charge polarization is successfully induced on the surface of melon‐based organic semiconductors by creating dual active sites with a large charge asymmetry. Confirmed by multiscale characterization and theoretical simulations, such asymmetric charge distribution, originated from the oxygen dopants and nitrogen vacancies over melon‐based organic semiconductors, reduces exciton binding energy and boosts exciton dissociation. The as‐formed charge polarization sites not only donate electrons to CO2 molecules but also accelerate the coupling of asymmetric *CO*CO intermediates for CO2 photoreduction into ethanol by lowering the energy barrier of this process. Consequently, an exceptionally high selectivity of up to 97% for C2H5OH and C2H5OH yield of 0.80 mmol g‐1 h‐1 have been achieved on this dual active sites organic semiconductor. This work, with its potential applicability to a variety of non‐metal multi‐site catalysts, represents a versatile strategy for the development of advanced catalysts tailored for CO2 photoreduction reactions.

Dual Active Sites with Charge-asymmetry in Organic Semiconductors Promoting C-C Coupling for Highly Efficient CO2 Photoreduction to Ethanol.

Selective CO2 photoreduction into high-energy-density and high-value-added C2 products is an ideal strategy to achieve carbon neutrality and energy shortage, but it is still highly challenging due to the large energy barrier of the C-C coupling step and severe exciton annihilation in photocatalysts. Herein, strong and localized charge polarization is successfully induced on the surface of melon-based organic semiconductors by creating dual active sites with a large charge asymmetry. Confirmed by multiscale characterization and theoretical simulations, such asymmetric charge distribution, originated from the oxygen dopants and nitrogen vacancies over melon-based organic semiconductors, reduces exciton binding energy and boosts exciton dissociation. The as-formed charge polarization sites not only donate electrons to CO2 molecules but also accelerate the coupling of asymmetric *CO*CO intermediates for CO2 photoreduction into ethanol by lowering the energy barrier of this process. Consequently, an exceptionally high selectivity of up to 97% for C2H5OH and C2H5OH yield of 0.80 mmol g-1 h-1 have been achieved on this dual active sites organic semiconductor. This work, with its potential applicability to a variety of non-metal multi-site catalysts, represents a versatile strategy for the development of advanced catalysts tailored for CO2 photoreduction reactions.

In Situ Synthesis of Copper-Based Metal-Organic Frameworks with Ligand Defects for Electrochemical Reduction of CO2 into C2 Products.

Electrochemical reduction of CO2 into high-value-added products is a potential approach to solving environmental problems but is limited by poor product selectivity and low efficiency. Metal-organic framework (MOF) materials have been considered one of the most promising catalysts, but their application is limited by complicated preparation processes, especially during the synthesis of organic ligands. In this work, a new three-dimensional Cu-MOF (JXUST-301) with high porosity was constructed based on the naphthalene diimide (NDI) ligand. Furthermore, JXUST-301 with ligand defects (JXUST-301D) originating from the missing NDI unit was synthesized via an in situ reaction. The presence of ligand defects endows JXUST-301D with a better CO2RR performance with a FEC2 of 56.7% and a jC2 of -162.4 mA cm-2. Mechanistic studies revealed that the hierarchical pore structure and amino sites are created from the absence of the NDI unit, which promotes the exposure of catalytically active sites and CO2 enrichment. Furthermore, the electronic structure of the Cu sites is modulated to upshift the d-band center, facilitating chemical adsorption and activation of key reaction intermediates. This work provides new insight into the in situ preparation of efficient Cu-MOF catalysts by introducing defects for the CO2RR.

Boosting the Efficiency and Selectivity of Electrocatalytic Reduction of CO2 to C1 Products by Mn-Porphyrin via Axial Ligation

Boosting the Efficiency and Selectivity of Electrocatalytic Reduction of CO₂ to C1 Products by Mn-Porphyrin via Axial Ligation