Even though global consensus has been reached in the Paris Agreement to limit global temperature rise to 2.0 °C, while pursuing efforts to limit the rise to 1.5 °C, recent analysis showed that it is likely that the 1.5 °C rise may be exceeded by the year 2027^[1]. It has also been reported that extreme climate incidents are occurring at a higher frequency in various parts of the world, which are closely related to climate change^[2]. Hence, decarbonisation efforts have to be more aggressive in the coming years in order to abate the ever-challenging effects of climate change.

Apart from conventional CO₂ mitigation measures such as energy efficiency improvement and adoption of renewables, the IPCC^[3] has proposed the adoption of carbon dioxide removal through negative emission technologies (NETs). The latter include emerging techniques such as enhanced weathering (EW), direct air capture, biochar, bioenergy with carbon capture and storage, etc.^[4,5]. NETs have several advantages over traditional decarbonisation measures; they allow the removal of historical CO₂ emissions and offset positive emissions from sectors that are hard to decarbonise, e.g. transportation, agriculture, etc. Note, however, that large deployment of NETs is associated with various financial and technical challenges^[4]. Hence, careful evaluation of NET deployment is necessary.

To allow large-scale deployment of NET in the near future, various systematic planning tools are necessary. Some of the process systems engineering and process integration tools developed in the past decades are believed to play a major role in large-scale deployment of CCS. One such promising tool is carbon emission pinch analysis (CEPA), which was first proposed for the optimal allocation of fossil and low-carbon energy resources in a carbon-constrained energy planning problem^[6]. The main underlying principle of CEPA is rooted in process integration, i.e., performance setting prior to detailed design. In the past four decades, process integration tools have been well established and dedicated to various industrial resource allocation problems, such as energy conservation^[7,8], material recovery^[9,10], etc. In the seminal work of CEPA, a graphical tool of carbon emission pinch diagram was proposed to locate the minimum amount of low-emission renewables while subject to the maximum CO₂ emission limit^[6]. Various successful applications have been reported worldwide, such as those in America^[11,12], Europe^[13-17], Asia^[18-20] and Oceania^[21,22]. In each of these applications, CEPA methodologies were tailor-made to account for local conditions. For instance, in the case of Poland, CEPA was used to set realistic renewable targets in phasing out lignite and hard coal, as the earlier energy plan did not account for the growing number of electric vehicles in the country^[17]. For the case of Bangladesh, Tarequzzaman et al.^[20] outlined strategies to facilitate Bangladesh’s long-term energy plan, in order to achieve the intended nationally determined contributions emission limit.

In recent years, various extended works of CEPA have been reported. In general, these extensions were meant to address greenhouse gas and CO₂ emissions in various settings. An important extension was reported by Tan et al.^[23], where a graphical targeting tool was used for optimal deployment of NETs such as EW and bio-char networks. Besides, Mu et al.^[24] integrated the concept of CEPA into a process graph in order to identify a raw material network of lower CO₂ emissions. Another work on lowering CO₂ emissions was reported by Zhang et al.^[25], who applied CEPA principles for the tobacco industry. On the other hand, Chew et al.^[26] made use of CEPA principles to optimise waste treatment system configurations while considering greenhouse gas reduction. In the work of Yang et al.^[27], a modified CEPA pinch diagram was used to compare the different options of coastal ecosystems (such as mangrove forests, seagrass beds, and coral reefs).

In this work, the EW network synthesis problem is analysed. A novel algebraic targeting tool, along with its automated targeting variant, is proposed for the analysis. These newly extended tools allow rapid determination of rigorous network targets due to their numerical nature, hence overcoming cumbersome manual plotting and inaccuracy issues that are inherent in the graphical method^[23]. The algebraic tool is highly welcomed as it may be implemented in spreadsheet software, which promotes its widespread usage among practitioners. In addition, the algebraic and automated targeting tools allow the generation of a new graphical tool, which facilitates analysis and discussion. Besides, this work is extended to single- and multiple-region problems. In the latter, sinks and sources of different regions may be allocated across the geographical border. These are the main novelties of this work, which complement the state-of-the-art of the current EW work.

The paper is structured as follows. In the following section, the problem statement for a terrestrial CMN is first given. Next, the basics of graphical targeting tools are explained. The newly proposed algebraic targeting method is next proposed, which is followed by its illustration in Example 1, which is a single-region problem. The algebraic targeting method is next extended into its automated targeting variant, which is then illustrated using Example 2, where an inter-region problem is solved. The paper is finally concluded and future research directions are suggested.

The problem for synthesising a terrestrial CMN can be stated as follows^[23]:

• Given CO₂ sources i, which are mineral crushing plants with known annual production capacity (f_SRi) and operating life (t_SRi). The product of the two parameters is the CO₂ output of each source (m_SRi).

• Given n CO₂ sinks, which are application sites with known annual (f_SKj) and application rate limit (m_SKj). Dividing the latter with former yields the minimum operating life of the sinks (t_SKj).

The problem may be represented as a superstructure where CO₂ sources are to be paired with CO₂ sinks, as shown in Figure 1. The main assumption of this synthesis problem is that all sources and sinks available for pairing will commence their operation at the same time^[23]. In other words, time constraints are not considered in the pairing problem.

In this work, the main objective is to identify the capacity deficit and excess capacity targets of the terrestrial CMN by considering intra- and inter-region applications. For the former, all sinks and sources are located within a close distance, and hence the crushed mineral may be sent from plants (sources) to the application sites (sinks) within the same region. In another scenario involving inter-regional applications, various sources and sinks are found in separate regions (e.g., city, province) which are further from each other. For the case of inter-regions, CO₂ sources may be sent to CO₂ sinks within the same region, before they are sent to sinks in another region; doing so will maximise carbon sequestration, with reduced excess capacity deficit and excess CO₂ load in the individual regions.

The algebraic tool has the following steps:

1. The sinks and sources are arranged in descending order of their operating life.

2. The application rates of the sinks (f_SKj) and sources (f_SRi) are added to form their cumulative values, i.e., Cum. f_SKj and Cum. f_SRi, respectively.

3. All cumulative application rates are then arranged in ascending order, with duplicates removed. These cumulative rates become the levels of the EW cascade and they are indicated as level k (Cum. f_k); a generic form of these cumulative rates is shown in column 1 of Table 1.

4. In column 2 of Table 1, the interval rates (∆f_k) are calculated as the differences of the adjacent levels k, as follows

(1) $$ \Delta f_{k}=\text { cum. } f_{k}-\text { cum. } f_{k-1} \\ $$

5. Within each interval, the sinks and sources are first located in columns 3 and 4, respectively.

6. Next, the interval capacities of the sinks (∆m_SK,k) and interval load of the sources (∆m_SR,k), are calculated using Equations 2 and 3, respectively. These values are documented in columns 5 and 6, respectively.

(2) $$ \Delta m_{\mathrm{SK}, k}=m_{\mathrm{SK} j} \frac{\Delta f_{k}}{f_{\mathrm{SK}, k}} \\ $$

(3) $$ \Delta m_{\mathrm{SR}, k}=m_{\mathrm{SR} i} \frac{\Delta f_{k}}{f_{\mathrm{SR}, k}} \\ $$

7. In column 7, the net capacity between the sinks and sources within each interval (r_k) is calculated using

(4) $$ r_{k}=\Delta m_{\mathrm{SR}, k}-\Delta m_{\mathrm{SK}, j} $$

A positive value indicates that the CO₂ sources are sufficient to meet the demand in the interval; a negative value means that the demand is not fulfilled.

8. The net capacity values are then accumulated downwards to form the capacity cascade in column 8, as follows

(5) $$ \mathrm{Cum.}\,r_k = \begin{array}{ll} 0 & k=1 \\[1pt] \displaystyle\sum_k r_k & k\geq 2 \end{array} $$

For a feasible capacity cascade, all net capacity values have to be positive, or at least zero - indicating that CO₂ sink capacity is large enough to capture the CO₂ load from the sources. If negative value(s) are observed, the capacity cascade is considered infeasible; Step 9 is to be followed.

9. The feasibility can be restored by identifying excess capacity (r_EC) of the CO₂ sink; the latter is identified with the largest deficit among the cascaded values in column 8.

(6) $$ r_\mathrm{D F}=\left|\min _{k} r_{k}\right| \\ $$

10. The absolute value of the largest deficit is returned as the Cum. r₁ value, located at the highest level in the EW cascade. The revised EW cascade will have all positive cascaded values, with zero value(s) indicating the pinch point of the sink-source matching problem, and may be viewed as the bottleneck of the CO₂ capture capacity. The last entry of the revised EW cascade indicates the excess or uncaptured load (r_LD) of the CO₂ sources.

(7) $$ \mathrm{Cum.}\,r_k = \begin{array}{ll} r_\mathrm{DF} & k=1 \\[1pt] \displaystyle\sum_k r_k & k\geq 2 \end{array} $$

11. Lastly, the cumulative carbon dioxide removal (Cum. CDR) can be calculated by multiplying the summation of carbon sequestration factor (α) and the CO₂ footprint per unit crushed rock allocated from source i to sink j (β_ij) with the total amount of rock supply from sources to sinks (R), as follows:

(8) $$ \text { Cum. } C D R=\left(\alpha+\beta_{i j}\right) R \\ $$

(9) $$ R=\sum_{j} m_{\mathrm{SK}j}-r_\mathrm{EC}=\sum_{i} m_{\mathrm{SR} i}-r_\mathrm{LD} \\ $$

Note that the summation of α and β gives the net carbon dioxide balance per unit of rock. Generally, the α value is negative and is substantially larger than β (Tan and Aviso, 2019)^[29]. In this work, the values of α and β_ij are taken as mean values reported in the literature. In actual implementation, their values may vary depending on factors such as particle size distribution, environmental conditions (pH, temperature, moisture), which affect the α value, as well as crushing, transportation, etc., that affect the β value. However, the methodology proposed in this work is based on process integration philosophy where the network performance targets are set in advance in priority to detailed analysis. This is in line with other process integration works such as heat recovery^[7,8], water minimisation^[8,9], property integration^[9], etc.

The advantage of the EW cascade is that column 1 (Cum. f_k) can be plotted against column 9 (Revised Cum. r_k) to form the GCC [Figure 3]; the latter provides visualisation on the sink-source matching problem. Due to the algebraic nature of the procedure, the GCC construction is much simpler as compared to the plotting of GCC from the composite curve [Figure 2A].

The automated targeting model (ATM) was established based on pinch analysis concept but is implemented on an optimisation platform. Hence, it possesses advanced targeting capabilities over traditional CEPA approaches. In this section, the ATM is extended to the EW network, for cases involving single- and multiple-regions.

A generic framework of the ATM is given in Figure 6. As shown, the latter has a similar structure to the algebraic targeting method. Hence, Steps 1-6 of the ATM remain identical to those of the algebraic method, while its remaining steps are given as follows. Note that step 6 has different variants for EW networks of single- and multiple-region.

7a. For EW of a single region, the residual capacity of every interval k (δ_k) is calculated from the net capacity between the sinks and sources, as well as the residual value cascaded from the earlier interval (δ_k-1), as determined using Equation 10 that follows

(10) $$ \delta_{k}=\delta_{k-1}+\left(\Delta m_{\mathrm{SR}, k}-\Delta m_{\mathrm{SK}, k}\right) \quad \forall k \\ $$

7b. For an EW network with multiple regions, Equation 10 is modified to consider import and export CO₂ load across different regions at every interval k.

(11) $$ \delta_{k}=\delta_{k-1}+\left(\Delta m_{\mathrm{SR}, k}-\Delta m_{\mathrm{SK}, k}\right)+\left(\sum_{q} \Delta m_{\mathrm{IM}, q, p, k}-\sum_{q} \Delta m_{\mathrm{EX}, p, q, k}\right) \quad \forall k \quad \forall p \\ $$

where ∆m_IM,q,p,k is total CO₂ load imported from region q into region p, while ∆m_EX,p,q,k is total CO₂ load exported from region p to region q.

8. The ATM is considered feasible when all δ_k values are zero or positive values, as all CO₂ load flows should be non-negative values, given as in

(12) $$ \delta_{k} \geq 0 \quad \forall k \\ $$

9. Set the objective of the problem. The latter may be set to minimise the excess capacity for a single-region problem, i.e.:

(13) $$ \min r_{\mathrm{EC}}=\delta_{0} \\ $$

For the inter-region problem, a two-stage optimisation approach may be adopted. In stage 1, the objective in Equation 13 is revised so that the overall excess capacity across all regions p is minimised:

(14) $$ \min r_{\mathrm{EC}}=\sum_{p} \delta_{p 0} \\ $$

In stage 2, the overall excess capacity determined in stage 1 is added as a new constraint as in Equation 15, while the objective is set to minimise the total cross-regional flows of CO₂ load across all levels among all plants (r_CP), given as in Equation 16. In practice, sending the CO₂ sources to sinks in other regions indicates that CO₂ emissions will be incurred from transportation. Hence, minimising cross-regional flows of CO₂ load will lead to reduced transportation emissions. The main assumption here is that transportation emissions are taken as the main factor in the inter-region problem.

(15) $$ r_{\mathrm{EC}}=r_{\mathrm{EX}, \text { Max }} \\ $$

(16) $$ \min r_{\mathrm{CP}}=\sum_{p} \sum_{q} \sum_{k} \Delta m_{\mathrm{IM}, q, p, k} \\ $$

10. Similar to the single-region concept, the cumulative CDR for all regions (Cum TSCDR) and the total amount of rock supply from sources to sinks can be calculated using

(17) $$ Cum TSCDR=\sum_{p}\left(\alpha_{p}+\beta_{i j p}\right) R_{p} \\ $$

(18) $$ R_{p}=\sum_{j} m_{S K j p}-r_{E C_{p}}=\sum_{i} m_{\mathrm{S R} i p}-r_{\mathrm{LD}_{p}} \\ $$

where α_p is the carbon sequestration factor for region p measured in CO₂ removal per unit of crushed rock applied, β_ijp is the CO₂ footprint per unit of crushed rock allocated from source i to sink j for region p, R_p is the total amount of rock supply from sources to sinks and, r_ECp and r_LDp are the excess capacity and excess CO₂ load of region p, respectively.

In this work, new pinch analysis tools were extended for EW problems. A new algebraic targeting tool was extended to overcome the limitation of the graphical method. Moreover, automated targeting method was extended for single- and multiple-region problems. Both tools may be used to plot the GCC, which is a useful visualisation tool for the sink-source matching problem. Two case studies, single- and multiple-region problems, were solved to elucidate the newly extended methods, along with the EW network design. Future work may focus on data uncertainties due to the risk of soil contamination in EW application. Site-specific weathering rates and process-related emissions may also be incorporated. Besides, temporal and multi-period considerations may also be incorporated.